In this study, a comparison between femtosecond (fs) and picosecond (ps) laser ablation of electrolytic iron was carried out in ambient air. Experiments were conducted using a Ti:sapphire laser that emits radiation at 785 nm and at pulse widths of 110 ps and 130 fs, before and after pulse compression, respectively. Ablation rates were calculated from the depth of craters produced by multiple laser pulses incident normally to the target surface. Optical and scanning electron microscopy showed that picosecond laser pulses create craters that are deeper than those created by the same number of femtosecond laser pulses at the same fluence. Most of the ablated material was ejected from the ablation site in the form of large particles (few microns in size) in the case of picosecond laser ablation, while small particles (few hundred nanometers) were produced in femtosecond laser ablation. Thermal effects were apparent at high fluence in both femtosecond and picosecond laser ablation, but were less prevalent at low fluence, closer to the ablation threshold of the material. The quality of craters produced by femtosecond laser ablation at low fluence is better than those created at high fluence or using picosecond laser pulses.