To increase the bond strength of CAD/CAM-fabricated, leucite-reinforced glass ceramics with a resin cement, the effects of the following were investigated: surface modification by tribochemical (TBC) treatment, followed by combined application of a silane coupling agent and a functional monomer as a primer. Bond strength was evaluated by a shear bond test. It was found that a silane coupling agent was useful for all the surfaces, particularly for the TBC-treated surface. This was because of the presence of a silica layer on the modified surface. The combination of a silane coupling agent and a functional monomer on the TBC surface allowed marked improvement in bonding, whereby the bonding endured 20,000 cycles of thermal cycling. Therefore, TBC treatment in combination with a silane coupling agent and a functional monomer as a primer substantially increased the bond strength of CAD/CAM-fabricated glass ceramics with resin cement, if the treatment conditions were appropriate.