The buffer leakage phenomena have a large effect on high‐power and fast‐switching GaN high electron mobility transistor devices. Herein, the buffer leakage mechanism in a GaN‐on‐Si substrate with AlGaN buffer layers is investigated by using samples with various carbon concentrations. Comparing the leakage current with crystallinity and impurity concentration, it is found that the vertical leakage current is dominated by both threading dislocations and bulk impurities. Increasing the carbon concentration of buffer layers suppresses leakage current in the bulk conducting regime in high electric fields but increases it in the dislocation conducting regime in low electric fields. These results indicate that the optimal carbon concentration of buffer layers depends on the target electric field.