The mechanochemical ball milling followed by heating at 650 °C for 5 h successfully produced the single-phase Bi2VO5.5powder. Catalytic activity for methylene blue dye degradation was investigated. Raman spectroscopy and X-ray diffraction were used to confirm the phase formation. The sample’s charge carrier transportation behavior was ascertained using time-dependent photocurrent analysis. The piezo-photocatalysis experiment yielded a 63% degradation efficiency for the ball-milled Bi2VO5.5sample. The pseudo-first-order kinetics of the piezo-photocatalytic dye degradation are discerned, and the significant k value of 0.00529 min−1is achieved. The scavenger test declares the h+radical is the predominant active species during the piezo-photocatalysis experiment. Vigna radiata seeds were used in a phytotoxicity test to evaluate the germination index. The mechanochemical activation method facilitates reactions by lowering reaction temperature and time. The effect of improved piezo-photocatalytic efficiency on the ball-milled Bi2VO5.5powder is an unexplored area, and we have attempted to investigate it. Here, ball-milled Bi2VO5.5powder achieved improved dye degradation performance.