I live in Natchitoches and teach at Northwestern State University, which may at the site of the "Catholic College" you are looking for. I see that your query was posted some time ago, but because my ancestors were from other places and I do my reseach in those areas, this is my first time to look at this web page.
Natchitoches was established on the Red River in 1714, and as such is an older town than New Orleans, San Antonio, and other towns in the Louisiana Purchase. Its entire old downtown area is federally designated as an historic district.
The St. Mary's Catholic School is a thriving elementary and secondary institution. Its first location was on a hill in the downtown area, just three streets back from the Red River (now Cane River Lake). After that structure burned, a modern brick structure was built several blocks away on the other side of Cane River.
Northwestern State University, where I now teach, was established in 1884 on the 900-acre grounds of a former plantation owned by the Bullard family. In 1856, the Bullard family had given the land to the church and the mansion was in use as a convent by the Religious of the Society of the Sacred Heart. In 1857 a school building was built at the convent. I don't know if that was the "college" in 1863, but it seems likely.
The only thing that remains of the mansion are three of the four columns that supported the east gable. Northwestern uses the three columns in its logo. Have a look at www.nsula.edu
Hope this helps.
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