In this article, we report the synthesis, structures, morphologies, and electrochromic properties of covalently bonded polyaniline (PANI)−TiO2 hybrids. The hybrids were synthesized via a sol−gel process, followed by oxidative polymerization, using a bifunctional compound to bridge the two phases. In comparison with PANI, the hybrids show significant enhancement in optical contrast and coloration efficiency. Furthermore, when covalently bonded to PANI, the TiO2 nanodomains can act as electron acceptors, reducing the oxidation potential and band gap of PANI, and improving the long-term electrochromic stability.