The authors report the results of investigating two models for ion-beam-induced deposition (IBID). These models describe IBID in terms of the impact of secondary electrons and of sputtered atoms, respectively. The yields of deposition, sputtering, and secondary electron emission, as well as the energy spectra of the secondary electrons were measured in situ during IBID using (CH3)3Pt(CPCH3) as functions of Ga+ ion incident angle (0°–45°) and energy (5–30 keV). The deposition yield and the secondary electron yield have the same angular dependences but very different energy dependences. It was also found that the deposition yield per secondary electron is very high (?10). However, within the investigated angle and energy ranges, the deposition yield is linearly related to the sputtering yield, the offset of which might be due to the contribution of primary ions. They conclude that the sputtered atom model describes IBID better than the secondary electron model.