Metalloid nanoparticles (MNPs) possess unique physicochemical properties but are challenging to create through biological or chemical routes. Using Pulsed Laser Ablation in Liquid (PLAL), Mg–C MNPs are fabricated from powders. The produced nanocolloids were ablated after the target was removed to tailor the particle size. MNPs with a mean size 300 nm could be reduced to 60 nm. Alternatively, MNPs with a mean size of 60 nm could be increased to 90 nm. The increase/decrease in size is controlled by the laser processing parameters and showcases the ability of PLAL for real-world applications that require meticulous control of size. The as-fabricated nanocolloids were successfully inkjet printed on paper, achieving a low resistivity of 75 Ω/square after 60 prints, highlighting their potential in printed electronics. To address a historical research gap, this article explored the impact of PLAL processing parameters, including fluence (1–2 J/cm2), pulse width (0.2–0.9 ns), repetition rate (10–20 kHz), and pH, factors often overlooked which is partly limiting applications. The influence of powder vs rod target on the PLAL process was addressed revealing that powders produce better size control and are easier to handle but they produce lower colloid concentrations.