Baltacha came from behind in both sets to wear the world number 135 down in under two hours and reclaim the title she held in 2011.
Her last tournament win at the Nottingham Tennis Centre was also the last time she clinched a title.
It was an emotional triumph for the 29-year-old, who spent more than eight months out of the game and came close to calling it quits.
"There is something about Nottingham, this is the third time I've won a title here and I've never lost a final,” she said.
“It is a very, very special place - it is magic for me to be honest.
"It means absolutely everything to me. I was pretty much bawling my eyes out.
"To think I actually nearly retired after the Olympics nearly a year ago. To then have ankle surgery, then go through rehab, I can’t believe how far I’ve come in such a short space of time. Having already scored two top 100 wins is incredible and now I’ve got this title.
"To come back and play tennis like that, consistently in five matches this week, was such amazing feeling – it is such a special win.”
The Aegon Team GB Fed Cup star called on every good omen she could in the first set as she struggled to contend with Majeric’s combination of stunning winners, sleek court movement and knack for producing the unbelievable.
From double faulting the first serve of the match, Baltacha failed to hold her first three service games. Her only response was to break the Slovenian to make it 1-3, and even then Baltacha dropped her next service game.
It wasn’t until Majeric was 5-1 up that the Scot finally held her first serve.
The Slovenian was then broken as she served for the first set. Baltacha fought on, saving two set points at 3-5, and then blitzed the 22-year-old to claim the see-sawing set 7-5.
Whatever momentum Baltacha thought she had at that stage was ripped from her as Majeric then broke the Brit in the first game of the second set.
The seventh seed held service before Baltacha wrestled the match back in her favour, going 5-2 up in another blistering display. At 5-3 up, Baltacha served for the match for the first time, and twice had championship point snatched from her by the unrelenting Majeric.
The Slovenian clawed her way back from the brink once again, taking the set to a tiebreak.
Neither one of them managed to take control early. The Slovenian had one set point at 6-5 in a see-sawing spectacle that summed up the battle, before the world No. 217 sealed victory.
“It was so exciting to be part of something like that – credit to her because she was unbelievable out there,” Baltacha said.
"At this point of my comeback, a tough match like that is something I really needed - I needed to get pushed hard to find things out about myself.
"One of the things I’ve definitely picked up on is that I’m stronger - I'm mentally stronger, my heart seems to be bigger and my stomach can tolerate much more now, which is exciting for me moving forward.
"I am going to Eastbourne and Wimbledon with the best form I possibly can. I couldn’t have had a better week getting ready for it."
Majeric, who fell in the first round of the Aegon Trophy at the same venue a week earlier, praised Baltacha’s fighting spirit.
“I played good out there, we both did,” Majeric said.
“It was a pretty interesting match - I was up 5-1 and lost the first set and then she was up 5-2 and I had a great comeback, but still she won it.
“I had my chances to win it, but still it has been a very good week for me heading into Wimbledon qualies.”