Later in 1852, he also worked as a bounty hunter, hunting for three mounted men seen in the area, thought to be the killers of Allen B. Ruddle, an unarmed young man robbed while traveling in a wagon to Stockton.

To earn the large reward for the capture of these men, put up by Ruddles family, Love and a partner, tracked the three riders to Rancho San Luis Gonzaga at the foot of Pacheco Pass then one of them with another man to Buenaventura in Santa Barbara County.

There in June 1852, they captured the one of two men they had followed, Pedro Gonzalez, later found to be a member of Joaquin Murrieta's gang, who had been accused of murder.

The unit was created on May 11, 1853 by Governor John Bigler specifically to capture or kill the "Five Joaquins" gang, who had been identified as being responsible for over 20 murders, and numerous robberies and horse thefts in California's Gold Country in just the early months of 1853.

From there they followed La Vereda del Monte to a point overlooking the Arroyo de Cantua, the gang's hideout and headquarters on July 21.

[5]: 473–475 On morning of July 25, 1853, Love and 20 of the Rangers encountered a small group of men south of Panoche Pass at the point where Arroyo de Cantua, emerged from the foothills, in Mariposa County, (in what is now Fresno County), about 100 miles (160 km) away from the Mother Lode and 88 miles (141 km) away from Monterey.

[6] The Rangers cut off the heads of both men as well as Garcia's hand as proof, sending them by fast riders ahead of the main force to Fort Miller.

Seventeen people, including a priest, signed affidavits identifying the remains as Murrieta's and Love and his Rangers received the reward money.

Harry Love's monument is located at the Mission City Memorial Park, 420 N Winchester Blvd., Santa Clara, CA 95050

In the film, after Joaquin's death, his (fictional) brother, Alejandro (Antonio Banderas), becomes the new Zorro and later kills Captain Love in revenge.

As he did in the movie, the actual Harry Love preserved Murrieta's head and Jack's hand in large, alcohol-filled glass jars.