We report on the frequency and stress dependence of the direct piezoelectric d33 coefficient in BiFeO3 ceramics. The measurements reveal considerable piezoelectric nonlinearity, i.e., dependence of d33 on the amplitude of the dynamic stress. The nonlinear response suggests a large irreversible contribution of non-180 domain walls to the piezoelectric response of the ferrite, which, at present measurement conditions, reached a maximum of 38% of the total measured d33. In agreement with this interpretation, both types of non-180 domain walls, characteristic for the rhombohedral BiFeO3, i.e., 71 and 109, were identified in the poled ceramics using transmission electron microscopy. In support to the link between nonlinearity and non-180 domain-wall contribution, we found a correlation between nonlinearity and processes leading to depinning of domain walls from defects, such as quenching from above the Curie temperature and high-temperature sintering. In addition, the nonlinear piezoelectric response of BiFeO3 showed a frequency dependence that is qualitatively different from that measured in other nonlinear ferroelectric ceramics, such as “soft” (donor-doped) Pb(Zr,Ti)O3 (PZT), i.e., in the case of the BiFeO3 large nonlinearities were observed only at low field frequencies (<0.1Hz); possible origins of this dispersion are discussed. Finally, we show that, once released from pinning centers, the domain walls can contribute extensively to the electromechanical response of BiFeO3; in fact, the extrinsic domain-wall contribution is relatively as large as in Pb-based ferroelectric ceramics with morphotropic phase boundary (MPB) composition, such as PZT. This finding might be important in the search of new lead-free MPB compositions based on BiFeO3 as it suggests that such compositions might also exhibit large extrinsic domain-wall contribution to the piezoelectric response.