Im going to start this answer with a bit of 'origin' history.

The French lost control of north-east Spain, then a defensive border region against Al-Andalus, in the chaos caused by the house of Capet replacing the house of Karling as rulers of France (the 990s). These border areas would, after enjoying a brief amount of time (historically) imdependent, they were brought under the control of Sancho the Great of Navarre (c. 992 – 18 October 1035), who for a brief time unified all of Christian Spain. When he died, the kingdom Sancho created broke up, and the result of this would eventually become what we now know as the kingdoms or 'Crowns' of Navarre, Aragon and Castile (this had largely happened by the 1100s). It is these states which interacted with France in the middle ages.

Navarre, thanks to its small size, focussed mainly on maintaining independence and opportunistic growth (it held counties in northern France at some points). Castile focussed mainly on expansion south in the Reconquista, managing its relations with Aragon to the east and the new Kingdom of Portugal, a strong ally of the King of England, to the west. Aragon also focussed on the Reconquista, but unlike Castile also expanded east into the Mediterranean, taking many islands such as Majorca, Ibiza and Sardinia. This reinforced Aragon's position in Spain as a more Venetian-like, trading nation in wat we now call a Thalassocracy. It also began to increase its interest in the northern Mediterranean coast, such as Marseilles in Provence (then a part of Germany/the HRE)but also important southern French towns such as Montpellier. This was made easier by the fact that southern French (actually Occitan), is remarkably close to the Catalan dominated Aragon culturally.

The French king, in the mean time, was becoming increasingly focussed on dealing with his vassals, notably the strongest, who was also at this point the King of England. And the entire history of French 'foreign policy' was epitomised in the Hundred years war, in which the King of England attempted to claim the throne of France (1337 to 1453).

As such Franco-Spanish relations were based on these England-France and Arago-Castilian dynamics. Aragon's desire to move into South-French, Occitan lands meant that an alliance with England in order to help make that happen. France then used Castile to maintain a counterweight in the south, similar to how it allied with Scotland in the Auld Alliance. This also put pressure on pro-English Portugal.

An example of this would be the Battle of Najera in 1367, where Edward Plantagenet of England, the 'Black Prince', fought a Castillian-French force in Northern Castile. The stake was the seat of the throne of Castile, and on one side was the incumbent Henry II Trastamara, supported by the French, while on the other side was the claimant Pedro the Cruel, who was supported by England and whose forces were led by the Black Prince. Though the battle as won by the the Black Prince, the war was won by Henry II, and as a result of this Castile agreed to support the French in their attacks on English held lands in southern France.

After this, most of the energies of Aragon and Castile would go south, into eliminating Al-Andalus in its entirety, which was achieved by 1492. Meanwhile, France ended the Hundred Years war with a decisive victory of the Kings of England, and began to focus on its most dangerous neighbour, the Ducky of Burgundy. After dealing with them in 1477, is cast its eye to Italy, the source of wealth in Europe and the soon to be flourishing Renaissance. This was an area which Aragon already had an interest in, as it controlled Sicily and Sardinia off the coast. By this point, Castile and Aragon has also largely set aside their differences and their two respective monarchs, Ferdinand II of Aragon and Isabella of Castile, had married beginning a process which would result in a unified Spain.

In order to secure control of southern Italy for France (a big French aim), Louis XII of France offered to divide the Kingdom of Naples between France and 'Spain' in what became known as the Treaty of Grenada. This was an important moment in history, as now 'Spain' had the 'right' to meddle in the politics of Italy, and sure enough Franco-Spanish relations quickly broke down. In the resulting war, 'Spain' was able to use its control of the Mediterranean and superior military tactics to decisively beat the French, taking full control of all of Italy south of Rome. In the next 'Italian wars', Spain would use its new-found position to exclude the French from Italy, with increasing levels of success. This was helped by the fact that the Spain was formally unified under its next King, the Hapsburg Charles V, who was also Emperor of the HRE.

These Italian wars were ended at the peace of Cateau-Cambresis in 1559 (where England also lost Calais to France), in which Spain was confirmed as overlord and protector of Italy and France was told to deal with it. Spain on the other hand was at its height, under Phillip II who was married to Mary I Queen of England, but nor Emperor of the HRE (they didn't elect him).

Sources can be provided on request (It might take a little while!)

tl;dr : They did a bit, but the Muslims were too interesting for the Spanish until the 16th century, and then they fought over Italy for a bit.