The disgruntled former prof previously filed a wrongful termination lawsuit against NYU in December, claiming that after he gave Franco the low grade - for allegedly missing 12 out of 14 classes - he was fired.
"Santana, as a full-time professor in the department, had every right to give such a grade to a student who failed to adequately attend and participate in his class," he charged in his suit at the time.
A rep for the uni branded Santana's lawsuit "ridiculous," adding, "It is regrettable and disappointing to see a faculty member - former or otherwise - discuss any student's grade for the purpose of his or her personal publicity."
After Santana was given the boot, Franco - who was later hired by the uni as a lecturer on how to adapt poetry into short films - had some harsh words for his former instructor.
"No teacher will ever be fired from NYU for giving a student a D," Franco had told reporters in April, according to ABC News.
"He wasn't fired, he was asked not to come back after three years because they didn't think he was a good teacher.
"I decided to do 127 Hours instead of going to acting class," he said.
"I've been in eight years of acting class. I didn't feel like I needed to waste my time with a bad teacher and that I should go and work with Danny Boyle. I felt like that was the right decision."
He continued: "I did not care one bit about the grade, I knew I was going to get the grade.
"I don't even know what my grades are in NYU because grades don't matter, what matters is the films that you make. Anybody coming out of film school is not going to go to Sony or Warner Bros and say 'Hey, I got an A in acting class, give me a job.'"
In an interview with the Post about the new lawsuit, Santana branded Franco a "bully" and said, "I didn't deserve to be on the receiving end of those falsehoods".
Adding: "I was outraged that someone with his attendance record at NYU had the audacity to make those statements."
Chimed Santana's lawyer, Matthew Blit: "When the suit was filed against him, Mr Franco initially took the high road and said nothing.
"Unfortunately, he could not help himself once his new movie [The Broken Tower] was being released."
Santana is seeking unspecified monetary damages, the Post reports.
No word as yet from Franco's rep on the lawsuit.
Fast gossip
And finally...
* Bradley Cooper opens up about road to sobriety; rumours he'll star opposite Beyonce in A Star is Born remake debunked.
* Mel Gibson's ex to get HUGE payout.
* Kim Kardashian says Kanye West her "perfect match".
* Britney Spears made the first move, says fiancé Jason Trawick.
* Katy Perry and John Mayer are back on...were they ever off?
* Angelina Jolie fires back at copyright infringement lawsuit.
* "I had to stand up for myself": Katherine Jenkins talks David Beckham affair rumours.
* Lady Gaga's new album ARTPOP to be launched as an app.
* Amanda Bynes charged with two counts of hit-and-run.
* Snooki shows off her baby boy Lorenzo.
* Shia LaBeouf opens up about split from Carey Mulligan.
* Michael Clarke Duncan's funeral details released.
* Will there be a director's cut of The Dark Knight Rises on Blu-ray?
* Alec Baldwin's daughter laughs off infamous "little pig" voicemail.
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