Sears said that he will teach three classes at Servite.
The Friars were 11-15 this year and didn't qualify for the playoffs.
"Laguna Beach was a great place," he said. "Everyday, I basically got to go to paradise to coach. But it was a challenge because there was a need to change the culture in the program.
"In my four years there, I saw tremendous growth from a young bunch of kids who were like sponges, who wanted to soak up and learn about baseball. The family atmosphere was tremendous. I had great support and that was a tremendous feeling. I'll take that with me."
Sears went 71-46 during his four years at Laguna. The 71 career wins is the most among the 26 coaches in the program's history. He holds the highest winning percentage and is tied with Norm Borucki for most career league wins (35).
"It was a one of those dream seasons," Sears said. "I was amazed by some of the feats these kids accomplished. Day in and day out, it seemed like a record was being broken.
"The kids will be upset with me for leaving and might not talk to me for a while, and I understand that. They realize what we had done and where the program was going. But I believe that this team will be really, really strong again next season. They're extremely good, extremely talented."
Laguna Beach Athletic Director and football Coach Mike Churchill said he has received "a lot of interest" in the now-vacant Laguna position. He said he posted the baseball job opening on Wednesday.
"After our season was over, several schools contacted Jeff," Churchill said. ""The Servite job was open and Jeff applied.
"This is a good break for him. He'll be coaching in the Trinity League, which has tough competition. He'll do a great job, I know. Their gain is our loss.
"Jeff and I came to Laguna Beach High at the same time. He made a commitment to the program and is an old-school guy who wanted things done his way. He got a group of kids who believed in what he was doing. …We're going to miss him. We'll find the best replacement that we can."