This paper presented a novel method for the organic pigment coated with titania to improve the weatherability and dispersion ability in waterborne system. The organic pigment was first orderly adsorbed by two kinds of electrolyte: poly(sodium 4-styrenesulfonate) (PSS) and poly(diallyldimethylammonium chloride) (PDADMAC), then coated by titania via sol-gel process from titanium n-butoxide (TBOT). The effects of the numbers of polyelectrolyte layer, water content, and TBOT content on the morphology, particle size, surface element composition, porosity and pore size, thermal stability, and UV shielding property of the organic pigment were systematically investigated. It was found that only two layers of electrolyte adsorption and one-step coating of titania could obviously enhance the UV shielding property even thermal stability of the organic pigment. The thickness of the titania layer could be easily tailored by TBOT content.