The Museo de Santa Cruz occupies a stunning 16th-century hospital building just off Plaza de Zocodover, the main square. The Plateresque facade — covered in carved stone ornament so delicate it looks like metalwork — is one of the finest in Spain. Inside, the museum's collection spans Roman mosaics, Visigothic stonework, medieval ceramics, tapestries, and paintings, with a particular strength in El Greco.
The layout follows the original hospital plan: a Greek-cross floor plan with a central space open to the sky, and galleries on two levels. The space itself is as interesting as the objects. Look for the El Greco Assumption of the Virgin in the main hall — it's one of his largest and most dramatic works, painted for the church of Santo Domingo el Antiguo and later moved here.
Admission is free, making this one of the best-value stops in Toledo. It is also less crowded than the Cathedral or the Alcázar, so if you need somewhere to rest mid-afternoon, the cool halls and calm patios are ideal.