$(Na_{0.525}K_{0.4425}Li_{0.0375})(Nb_{0.9975}Sb_{0.065}Ta_{0.0375})O_3+0.3 wt%CoO$ ceramics were fabricated as a function of CuO addition by traditional solid state sintering process in order to develop excellent lead-free piezoelectric ceramics composition. The addition of CuO in the LNKNTS composition ceramics can effectively enhance the densification of the ceramics, resulting in the oxygen vacancies as hardening effect. The excellent piezoelectric properties of electromechanical coupling factor($k{small}_P$) of 0.378, piezoelectric constant($d_{33}$) of 152 pC/N were obtained from the 1.0 mol% CuO doped LNKNTS ceramics sintered at $1,020^{circ}C$ for 3 h.