Conductive fillers, such as amorphous carbon, carbon nanotube and graphene etc., are generally mixed with nanostructured metal oxide materials to improve the performance of electrode materials in energy storage devices. However, the conductive framework that provides path for electric conduction does not normally form a well-connected and robust 3-D network to ensure optimized ions transport. Here, we report a convenient, inexpensive and scalable method for synthesizing hybrid carbon and titanium dioxide co-gels and co-aerogels to improve the electrochemical capacity by combining both the lithium insertion and the surface storage mechanisms in Li ion batteries (LIBs) anodes. A monolithic piece of a hybrid C/TiO2 co-aerogel can be directly used as an active electrode without the addition of binders, such as polyvinylidene fluoride (PVDF). As a result, the performance of LIB anodes using the hybrid co-aerogel is significantly improved over current LIBs based on carbon/titanium oxide composites. The reversible discharge capacity was stabilized at ∼400 mAh g−1 at a 168 mA g−1 scan rate and an operating voltage between 3.0 and 0.05 V vs. Li+/Li with excellent cyclic capacity retention. This approach, however, is not limited to only C/TiO2 system but can be extended to other metal oxides to form co-gels with carbon to improve their potential use in numerous electrochemical, photocatalytic, and photoelectronic devices.