We present spectropolarimetric observations of the peculiar Type Ib/c SN 2005bf, in MCG+00‐27‐005, from 3600–8550 Å. The SN was observed on 2005 April 30.9, 18 d after the first B‐band light‐curve maximum and 6 d before the second B‐band light‐curve maximum. The degree of the interstellar polarization (ISP), determined from depolarized emission lines in the spectrum, is found to be large with pmax(ISP) = 1.6 per cent and , but this may be an upper limit on the real value of the ISP. After ISP subtraction, significant polarization is observed over large wavelength regions, indicating a significant degree of global asymmetry, ≳10 per cent. Polarizations of 3.5 and 4 per cent are observed for absorption components of Ca ii H& K and infrared triplet, and 1.3 per cent for He i 5876 Å and Fe ii. On the Q–U plane clear velocity‐dependent loop structure is observed for the He i 5876 Å line, suggestive of departures from an axial symmetry and possible clumping of the SN ejecta. Weak high‐velocity components of Hα, Hβ and Hγ are observed, with velocities of −15 000 km s−1. The low degree of polarization observed at Hβ suggests that the polarization observed for the other Balmer lines (∼0.4 per cent above the background polarization) may rather be due to blending of Hα and Hγ with polarized Si ii and Fe ii lines, respectively. We suggest a model in which a jet of material, that is rich in , has penetrated the C–O core, but not the He mantle. The jet axis is tilted with respect to the axis of the photosphere. This accounts for the lack of significant polarization of O i 7774 Å, the delayed excitation and, hence, observability of He i and, potentially, the varied geometries of He and Ca.