The substitution of Al for Ti simplified the preparing method of Ca0.35Li0.25Nd0.35TiO3 ceramics. BaCu(B2O5) was doped to reduce the sintering temperature of Ca0.35Li0.25Nd0.35Ti1-xAlxO3 ceramics. The Ca0.35Li0.25Nd0.35TiO3 ceramics with 3% mol Al2O3 and 5 wt% BaCu(B2O5) were sintered at 950 °C. The τf of BaCu(B2O5) doped Ca0.35Li0.25Nd0.35Ti1-xAlxO3 ceramics was in range of 65 ppm/°C to 41.2 ppm/°C. The optimal microwave dielectric properties were εr = 109.5 and Q × f = 2979 GHz.