To obtain the brazing effect of good exposure of abrasive particles and uniform thickness of the solder layer, the concept of vacuum brazing diamond with large particle size alloy solder was proposed, and the geometric model was established. The equation group of the relationship between large particle size alloy solder and diamond particle size was obtained, and the practical solution based on the wetting angle of alloy solder was obtained. In this study, NiCr alloy particles were used as the bonding agent and four sets of controlled experiments with different size combinations were conducted. The intermediate interface was analyzed by scanning electron microscopy and X-ray energy spectrometer. According to the test results, it demonstrated a large size NiCr alloy provides high consistency after brazing. Carbide chromium compound was also founded at the interface between diamond and alloy, which realized the firm control of diamond. This study showed that the new diamond brazing process based on the particle size matching mechanism was a feasible and promising method.