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The feasibility of CuP as a multifunctional additive in lithium grease was evaluated for the first time. The experimental results indicated that the CuP significantly enhanced the friction reduction, antiwear properties, extreme pressure capabilities, and antimicrobial characteristics of lithium greases. The SRV test results suggested that the optimal tribological properties were obtained by adding 3 wt% of CuP to lithium greases, resulting in a decrease of the friction coefficient and wear volume by 28.25% and 34.98%, respectively. The four-ball results confirmed that the extreme pressure performance of the lithium grease with 3 wt% CuP was enhanced by a factor of 3.17. The bacterial inhibition rate of lithium grease with 3 wt% CuP was higher than 99.98%. The lubrication mechanism and antimicrobial mechanism was explained.