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Smith is now accused of taking several sexually explicit pictures of his students. Police said the images - taken in 2011 and 2012 - were found on his computer.
The victims were 14 and 15 at the time. The girls were either fully or partially nude.
An ABC11 crew went to the school's Lead Mine Road location to see whether the administration would speak about the new allegations.
The school issued this statement:
"It is devastating to learn that one of our teachers has been charged with such serious crimes. Our hearts go out to the victims and their families. The Montessori School of Raleigh remains committed to protecting and supporting our students during this difficult time."
According to a bio on the school's website which has since been taken down, Smith taught at the school for 12 years and was the math director at the middle and upper school.
In November, Smith was charged with statutory rape and sex offense with a student.