The environmentally friendly additives were added into the optical variable ink, and the environmentally friendly printing ink suitable for various printing methods was made through compounding experiments. Three formulas were obtained by adjusting the quality ratio of the environmentally friendly optical variable ink. Then samples of the three kinds of ink were tested for printing adaptability by relevant means of detection and equipments, including ink fineness, viscosity, dryness, VOCs content and printing quality, etc.. The detection results showed that the fineness of the three ink samples was less than 20 μm, the time was 18.5~30.0 s, with good drying performance and low VOCs content. With the printing methods of screen printing, sheet fed gravure printing, and web gravure printing, the dried prints using the three kinds of ink possessed good green purple red light anti-counterfeiting effect, with the printed ink sample crack-free. Through optimizing, the optical variable ink demonstrated a variety of printing adaptabilities and environmental protection performances.