Ca_0.7La_0.2TiO₃ （CLT） was respectively hydroxylated （CLT—OH） by 30% H₂O₂ and modified （CLT—VT） by Trimethoxy（vinyl）silane （VTMS）. The hydrophilic and hydrophobic layers are respectively obtained on the ceramic surface， and they form hydrogen bonding and physical adsorption with the resin. By melt casting method， the modified ceramics and vinyl silicon-containing aryne resins （PSAE） were prepared into a series of microwave dielectric composite materials with different dielectric constants. The effect of different ceramic/resin interface forces on the properties of composite materials was studied. It was found that 40 vol%CLT—VT/PSAE achieved the best dielectric performance at 10 GHz， with a dielectric constant of 13.8 and a dielectric loss of 3.16×10^-3 and 40 vol%CLT—OH/PSAE has obtained the best overall performance， with a bending strength of 50 MPa， a dielectric constant of 14.77， and a dielectric loss of 3.29×10^-3.