In this work, a series of samples Ca3Ga4O9:0.01Bi3+,xTb3+(CGO:0.01Bi3+,xTb3+) were synthesized using high-temperature solid-state method. Their crystal structure, photoluminescence (PL), mechanoluminescence (ML) and thermoluminescence (TL) were investigated. Discovered that CGO:0.01Bi3+,xTb3+has the characteristic of dual emission. The waveform of mechanoluminescence emitted by CGO:0.01Bi3+,xTb3+under the action of loading mechanical force is similar to that of PL, indicating that the luminescent ions are Tb3+ions. And its mechanoluminescence has a good linear relationship and recoverability. The mechanoluminescence principle of CGO:0.01Bi3+, xTb3+is discussed by using first-principles calculations based on density functional theory (DFT), and a multi-mode anti-counterfeiting device with flexibility and rigidity is developed.