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Hey! A question right up my alley!
"Does the US Constitution allow for states to secede from the Union?" No, it does not, and that was the widely regarded opinion before the Civil War, at least up until the early 1830s, when hard-line Southern Democrats began talking increasingly openly about the possibility of secession.
Had U.S. law directly put it in writing that secession was illegal? No, but that's because the question had never directly come up in the courts, and the writers of the Constitution had taken it for granted that ratification of the Constitution would be "in toto and for ever" as James Madison wrote to Alexander Hamilton at the time the Constitution was being ratified by the states.
In fact, Madison wrote to Hamilton because some New York politicians were arguing at the time for a provision to be let out of the Constitution if they later changed their mind. Hamilton solicited Madison's advice, who told him that Virginia had considered a similar provision, but declined to adopt it, considering it not a true ratification, and worse than rejection. Hamilton then made the same argument at the New York convention. This led to New York ratifying the Constitution without reservations.
Through many different court rulings, the federal courts had given every indication that they would have almost certainly ruled against secession if the issue had been brought to the courts before the Civil War. It's the very reason why there was a war to secede, instead of a lawsuit to secede. If it were legal, then the Southern states could have saved a lot of time, effort, and blood by just suing the federal government for the enactment of their legal Constitutional rights. But the South didn't do this because the federal courts had a long history of ruling diametrically opposite to their point of view.
Perhaps the most important and one of the earliest federal cases that danced around the subject was the 1809 ruling United States v. Peters. This ruling decided unanimously that nullification of federal laws by the states was illegal. As Chief Justice John Marshall wrote in the court's opinion:
"If the legislatures of the several states may, at will, annul the judgments of the courts of the United States, and destroy the rights acquired under those judgments, the constitution itself becomes a solemn mockery; and the nation is deprived of the means of enforcing its laws by the instrumentality of its own tribunals."
This is important because, at its heart, secession is simply the nullification of all federal laws and not just one. The Supremacy Clause of the Constitution gives legal precedence over the states in regards to any federal law deemed Constitutional, and the states are Constitutionally obligated to abide by it. Just because the Southern states were trying to nullify all federal laws and not just one didn't really make much difference.
But the Constitution doesn't directly address "secession" or leaving the union in direct language. It does, however, infer what the nature of the "union" established under the Constitution means. The first sentence of the Preamble of the Constitution starts:
"We the people, in order to form a more perfect union..."
But "more perfect" than what? This was a reference back to the less-than-perfect "union" established under the Articles of Confederation which explicitly called it a "perpetual union." And that goes back to Madison's and others' writings at the time the Constitution was ratified, that it was meant to be a perpetual document that all the states were obligated to abide by. No exit could be accomplished short of going through the Constitutional process of passing an Amendment along the lines of, "The people of South Carolina are no longer party to the Constitution."
There was an opposite viewpoint to all this, however, which was called the "Compact Theory" of the Constitution. This was first advanced by early 19th Century federal appeals (not Supreme Court) justice St. George Tucker. In 1803, he wrote a treatise called View of the Constitution of the United States with Selected Writings in which he advanced the argument that the Constitution was a "compact" or contract between thirteen parties--the states--and any one of them had the right to pull out of the contract at any time they wished--on a single law or on all the laws. Never mind this is not how contracts typically work (try pulling out of your cell phone contract early, or nullifying some of the terms of the contract and see if the cell phone company has nothing to say about it), but it also ignores the fact that the Constitution is not established by thirteen parties. It is established by all the people of all the states, hence its first three words are, "We the people..."
Revealingly, despite the name of Tucker's book, the theory of a "voluntary compact" he expounds is mostly based on the author's reading not of the Constitution, but of the Declaration of Independence, a document based on "natural law" and not on the U.S. Constitutional law that was written more than a decade later. Tucker writes (emphasis mine):
"[We must not] forget that solemn declaration [i.e., the Declaration of Independence] to which every one of the confederate states assented. '…that whenever any form of government is destructive of the ends of its institution, it is the right of the people to alter or abolish it, and to institute new government.' Consequently whenever the people of any state, or number of states, discovered the inadequacy of the first form of federal government to promote or preserve their independence, happiness, and union, they only exerted that natural right in rejecting it, and adopting another, which all had unanimously assented to, and of which no force or compact can deprive the people of any state, whenever they see the necessity, and possess the power to do it."
In any case, the Supreme Court rejected Tucker's view of Constitutional law time and again, probably most forcefully in the 1816 decision Martin v. Hunter's Lessee. In the unanimous decision, Justice Joseph Story wrote against compact theory in his opinion for the majority:
"[T]he constitution of the United States...was ordained and established not by the states in their sovereign capacities, but emphatically, as the preamble of the constitution declares, by the people of the United States."
The rejection of the "Compact Theory" was again "forcibly stated" by the Supreme Court in the case of McCulloch v. Maryland in 1819. In that opinion, the court decided:
"The constitution, when thus adopted, was of complete obligation, and bound the state sovereignties."
Time and time again, the Supreme Court rejected any kind of advancement of a "Compact Theory" of the United States Constitution and any usurpation of Constitutional law by the states over federal supremacy. While none addressed secession directly, among many such relevant cases on the federal/state relationship were Ware v. Hylton (1796), Marbury v. Madison (1803), Fletcher v. Peck (1810), Cohens v. Virginia (1821), Gibbons v. Ogden (1824), Worcester v. Georgia (1832), and Ableman v. Booth (1859). These were all "state's rights" cases in some capacity or other, and the "states rights" side lost in all of them, almost always by a unanimous decision.
The "Compact Theory" advocates' position came down to two foremost arguments. One was, "Thomas Jefferson supported it." This was based on readings of several of Jefferson's writings, most thoroughly in a private letter he wrote in 1825, years after he'd been president. But, Jefferson was not a signer nor an author of the Constitution. He was in France while the document was drafted, passed, and ratified.
The other argument that the "Compact Theory" advocates relied upon was the text of a couple of resolutions passed in Virginia and Kentucky in 1798 referred to as the "Kentucky and Virginia Resolutions." These were both in response to the "Alien and Sedition Acts" passed by the federal government under John Adams. Neither resolution actually takes the position that the states have the right to nullify the law, but they take the position that they won't enforce the federal law. And if the feds have a problem with it, then they'll have to sue to get enforcement. Lucky for the Compact Theorists that it never came down to this. Adams was out of office and the laws were repealed before either Virginia or Kentucky was sued to try to enforce those federal laws.
Nonetheless, the burgeoning "Compact Theory"/"States Rights" movement in South Carolina began arguing on both these points at the time of the Nullification Crisis in 1831-32. As it so happened, James Madison was still alive at the time and wrote a lengthy rebuttal of this Southern position. Madison was not only called the "Father of the Constitution" but he also wrote the Virginia Resolution that the "Compact Theorists" were relying upon to make their argument. In rebuttal, Madison wrote that the Virginia Resolution was not a nullification, and only applicable to the Alien and Sedition Acts. It was, in fact, the start of an effort to possibly get the states together under the "state convention" method of amending the U.S. Constitution to overturn the Alien and Sedition Acts, if need be (which turned out to be unnecessary).