In this Letter, we report measurements of the coupling between Dirac fermion quasiparticles (DFQs) and phonons on the (001) surface of the strong topological insulator Bi2Se3. While most contemporary investigations of this coupling have involved examining the temperature dependence of the DFQ self-energy via angle-resolved photoemission spectroscopy measurements, we employ inelastic helium-atom scattering to explore, for the first time, this coupling from the phonon perspective. Using a Hilbert transform, we are able to obtain the imaginary part of the phonon self-energy associated with a dispersive surface-phonon branch identified in our previous work Phys. Rev. Lett. 107, 186102 (2011) as having strong interactions with the DFQs. From this imaginary part of the self-energy we obtain a branch-specific electron-phonon coupling constant of 0.43, which is stronger than the values reported from the angle-resolved photoemission spectroscopy measurements.