Acid Green 25 (AG25) has been cointercalated with Acid Yellow 25 (AY25) into the interlayer of ZnAl layered double hydroxides (LDH) via a coprecipitation method to tune the color of hybrid pigments based on LDHs. The prepared hybrids were analyzed by X-ray diffraction, scaning electron microscopy, Fourier transform infrared microscopy, inductively coupled plasma-emission spectroscopy, thermogravirnetry-differential thermal analysis, UV-vis, and CIE 1976 L*a*b* color scales, which show that AG25 and AY25 have been cointercalated into LDH and the color of the prepared LDH can be easily tuned from greenish blue to bluish green and green by adjusting the molar ratio of AY25/AG25. There exists host-guest and guest-guest interactions in the hybrids, and the intercalation into LDH significantly improves the thermal stability of the AY25. The hybrids were used as colorant to prepare green coatings and films, showing their potential application in the fields of paints and plastics.