When a few drops of acid (hydrochloric, acrylic, propionic, acetic, or formic) are added to a colloid comprised of 1D lepidocrocite titanate nanofilaments (1DLs)–2 × 2 TiO6 octahedra in cross‐section–a hydrogel forms, in many cases, within seconds. The 1DL synthesis process requires the reaction between titanium diboride with tetramethylammonium (TMA+), hydroxide. Using quantitative nuclear magnetic resonance (qNMR), thermogravimetric analysis (TGA), and differential scanning calorimetry (DSC), the mass percent of TMA+ after synthesis is determined to be ≈ 13.1 ± 0.1%. The TMA+ is completely removed from the gels after 2 water soak cycles, resulting in the first completely inorganic, TiO2‐based hydrogels. Ion exchanging the TMA+ with hydronium results in gels with relatively strong hydrogen bonds. The hydrogels' compression strengths increased linearly with 1DL colloid concentration. At a 1DL concentration of 45 g L−1, the compressive strength, at 80% deformation when acrylic acid is used, is ≈325 kPa. The strengths are ≈ 50% greater after the TMA+ is removed. The removal of all residual organic components in the hydrogels, including TMA+, is confirmed by qNMR, Fourier‐transformed infrared spectroscopy (FTIR), and TGA/DSC. The 1DL phase is retained after gelation, TMA+ removal, and 80% compression.