Amorphous indium-gallium-zinc oxide (a-IGZO) films, which are widely regarded as a promising material for the channel layer in thin-film transistors (TFTs), require a relatively high thermal annealing temperature to achieve switching characteristics through the formation of metal–oxygen (M–O) bonding (i.e., the activation process). The activation process is usually carried out at a temperature above 300 °C; however, achieving activation at lower temperatures is essential for realizing flexible display technologies. Here, a facile, low-cost, and novel technique using cellophane tape for the activation of a-IGZO films at a low annealing temperature is reported. In terms of mechanochemistry, mechanical pulling of the cellophane tape induces reactive radicals on the a-IGZO film surface, which can give rise to improvements in the properties of the a-IGZO films, leading to an increase in the number of M–O bonds and the carrier concentration via radical reactions, even at 200 °C. As a result, the a-IGZO TFTs, compared to conventionally annealed a-IGZO TFTs, exhibited improved electrical performances, such as mobility, on/off current ratio, and threshold voltage shift (under positive bias temperature and negative bias temperature stress for 10,000 s at 50 °C) from 8.25 to 12.81 cm²/(V·s), 2.85 × 10⁷ to 1.21 × 10⁸, 6.81 to 3.24 V, and −6.68 to −4.93 V, respectively.