TiO2 has attracted tremendous research interest for photocatalytic water splitting, solar hydrogen generation, environmental pollution removal, dye-sensitized solar cells, lithium-ion batteries, supercapacitors, and field emission. Microwave absorption materials (MAMs) play important roles in many military (e.g., the stealth coating on the B-2 bomber) and civil (e.g., telecommunications, noise reduction, information security, signal, and data protection) applications. However, TiO2 is not a good MAM due to its poor absorption in the microwave region. Here, we report that via hydrogenation excellent and tunable microwave absorption is achieved with hydrogenated TiO2 nanocrystals. After hydrogenation, 4.3x and 103x improvements have been obtained in storing and dissipating the electric energy of the microwave electromagnetic field. Their permittivity values are higher than those of the current carbonaceous MAMs. Instead of relying on the dipole rotation or ferromagnetic resonance mechanisms for traditional MAMs, the hydrogenated TiO2 nanocrystals work as good MAMs based on a newly proposed collective-movement-of-interfacial-dipole (CMID) mechanism. Although there is still no direct physical evidence of the interface effects of the CMID mechanism, the CMID as a hypothesis at this point successfully explained the origin of the enhanced microwave absorption of the hydrogenated TiO2 nanoparticles. This study thus may open new applications for TiO2 nanocrystals and also stimulate new approaches for new MAM development.