Within the context of reducing production costs, thin (<90 μm) silicon foils intended for photovoltaic applications have been fabricated from standard (100)Si wafers using a lowtemperature (<150 °C) stress-induced lift-off process. A multi-frequency electron spin resonance (ESR) study was performed in order to evaluate, at atomic scale, the quality of the material in terms of defects, including identification and quantification. Generally, a complex ESR spectrum is observed, disentangled as the superposition of three separate signals. This includes, most prominently (∼91% of total density) the D-line (Si 3 ≡Si• dangling bonds in a disordered Si environment), a set (∼6%) of highly anisotropic signals ascribed to dislocations (K1-like), and a triplet, identified as the Si-SL5 N-donor defect. Defect density depth profiling from the lift-off side shows all signals disappear in tandem after etching off a ∼33 μm thick Si layer, indicating a highly correlated−equal in relative terms−distribution of the three types of defects over the affected top part of the Si foil. The defect density is found to be highly non-uniform laterally, with the density peaking near the crack initiation point, from which defect generation spreads. It is thus found that the SLIM-Cut method for fabrication of thin Si foils results in the introduction of defects that would unacceptably impair the functionality of photovoltaic cells built on these substrates. Fortunately, this may be cured by etching off a thin top Si layer, resulting in a most useful thin Si foil of standard high quality.