Micro‐ and nanofibers produced by electrospinning and solution blow spinning (SBS) are highly suitable platforms for diverse applications due to their advantageous properties, including the high surface area to volume ratio, high porosity, and flexibility. To render them additional functionalities, distinct pre‐ or post‐modification processes have been proposed for modifying such micro‐ and nanofibers with 0D, 1D, 2D, and 3D nanostructures. The pre‐modification requires the addition of 0D–3D nanostructures (or their precursors) into the polymeric phase before the spinning process, which can demand laborious solubilization and requires changes in experimental spinning parameters, with impact on morphology, spinnability, and properties. Post‐modification methods, on the other hand, enable the fabrication of composite fibers without the need to optimize the spinning parameters, allowing a simple and efficient surface modification. Herein, recent advances on post‐modification methods of spun fibers, including wet chemistry, grafting, crosslinking, click chemistry, oxidations, hydrolysis and reduction strategies, dip‐coating, layer‐by‐layer, electro/air‐spray, atomic layer deposition, and plasma techniques aiming at the surface functionalization with 0D–3D nanostructures are surveyed. Recent results, trends, and challenges on the application of such surface‐modified fibers for environmental, industrial, and medical applications, including as adsorbent and filtering membranes, catalysts for pollutants degradation, and wearable sensors are examined.