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The couple first got engaged in 1950, but they lost track of each other when Harrod went off to serve in the Korean War.
"We've been in love for 59 years," said 75-year-old wife Fontelle Harrod.
Fontelle's daughter, who heard stories of her mother's first love, tracked down Harrod's phone number, and a reunion was arranged.
The couple finally married last month in Orange County.
But on Monday, while a son-in-law went to the hardware store, Harrod went missing.
Harrod's family says he took his wallet and keys, but left his car at home.
"We haven't seen any activity on his bank account, on his credit cards," said detective Corinne Loomis from the Placentia Police Department.
Harrod's new bride says she last spoke to her husband on Sunday.
"He was in very good spirits," she said.
Police have been going door-to-door in his neighborhood and are handing out flyers with Harrod's picture.
"Dad, if you're watching, come home. We're here, we're waiting, and your wife is waiting for you, and I love you dad," said daughter Julie Michaels.
Anyone with information is urged to call the Placentia Police Department at (714) 993-8194.