The polysaccharide FucoPol has recently been shown to yield hydrogel membranes (HMs) characterized by good mechanical properties, biocompatibility, and anti-inflammatory activity that render them promising biomaterials for use in the biomedical field. Subsequently to such findings, envisaging their development into novel delivery systems for topical applications, in this study, FucoPol HMs prepared by crosslinking the biopolymer with iron cations were loaded with caffeine or diclofenac sodium as model drugs. Two loading methods, namely diffusion and mixing, were applied to evaluate the FucoPol's HM drug-loading capacity and entrapment efficiency. The diffusion method led to a higher caffeine loading (101.9 ± 19.1 mg/g) in the HM1_D membranes, while the mixing method resulted in a higher diclofenac sodium loading (82.3 ± 5.1 mg/g) in the HM1_D membranes. The HM1_D membranes were characterized by increased mechanical and rheological parameters, such as their hardness (130.0 ± 5.3 kPa) and storage modulus (1014.9 ± 109.7 Pa), compared to the HM1_D membranes that exhibited lower values (7.3 ± 1.2 kPa and 19.8 ± 3.8 Pa, respectively), probably due to leaching occurring during the drug-loading process. The release profiles revealed a fast release of both APIs from the membranes loaded by diffusion, while a prolonged and sustained release was obtained from the membranes loaded by mixing. Moreover, for all API-loaded membranes, the release mechanism followed Fickian diffusion, with the release rate being essentially governed by the diffusion process. These findings, together with their previously shown biological properties, support the suitability of the developed FucoPol HMs to be used as platforms for the topical delivery of drugs.