Hendaye – Bayonne – Tarbes – Toulouse by train. SNCF / TER Aquitaine.
There is a direct Intercité train between Hendaye and Toulouse. There is also a TGV route, but this involves a change of trains at Bordeaux (Saint-Jean station), and bypasses the more-scenic route that will take you via Lourdes (so avoid this option if you want to stop there).
Instead, I took the even slower option of changing at Bayonne, onto a regional (TER) train, and then changed again at Tarbes onto yet another TER train, and then continued on to Toulouse (Matabiau station).
Much slower (stops everywhere), but when it comes to all things train travel, I love slow (more stations; more interaction with the locals; and more time to take in the wonderful scenery).
Web resources for this route:
Official Train Operator: www.sncf.com (English version)
Official Train Operator: www.ter.sncf.com/nouvelle-aquitaine (French)
The Perfect 3-Day Weekend in Toulouse (www.luxeadventuretraveler.com)
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[photo credit: commons.wikimedia.org]