Magnesium phosphate cement (MPC) is a potential substitute of epoxy as an adhesive material due to its advantages in setting time, early strength, and good fire and corrosion resistance. In this study, silica fume (SF) and calcium carbonate whisker (CCW) were employed to improve bond capacity of MPC which were used instead of epoxy in near-surface-mounted (NSM) fiber-reinforced polymer (FRP) systems. A direct pull-out test (DPT) was carried out to investigate bond performances of FRP–concrete interface after incorporating SF and CCW. According to the mix proportion of the MPC, a total of twenty-seven specimens in nine sets were divided into four groups: one group without additive, one group with SF alone, one group with CCW alone, and the last group with SF and CCW combination. Results showed that SF or CCW alone could improve MPC bond capacity, but their excess application would reduce it. SF and CCW combination, however, did not improve bond capacity as effectively as SF or CCW alone. Moreover, the addition of CCW would improve MPC’s bond ductility, with or without the adding of SF, but with the increase in CCW concentration, this improvement effect would decrease. Meanwhile, SF alone lowered its bond ductility.