Environmental pollution with cadmium (Cd) is a major concern worldwide, with prolonged exposure to this toxic heavy metal causing serious health problems, such as kidney damage, cancer, or cardiovascular diseases, only to mention a few. Herein, a gold-coated reflection-type fiber optic–-surface plasmon resonance (Au-coated FO-SPR) sensor is manufactured and functionalized with (i) bovine serum albumin (BSA), (ii) chitosan, and (iii) polyaniline (PANI), respectively, for the sensitive detection of cadmium ions (Cd2+) in water. Then, the three sensor functionalization strategies are evaluated and compared one at a time. Out of these strategies, the BSA-functionalized FO-SPR sensor is found to be highly sensitive, exhibiting a limit of detection (LOD) for Cd2+ detection at nM level. Moreover, the presence of Cd2+ on the FO-SPR sensor surface was confirmed by the X-ray photoelectron spectroscopy (XPS) technique and also quantified consecutively for all the above-mentioned functionalization strategies. Hence, the BSA-functionalized FO-SPR sensor is sensitive, provides a rapid detection time, and is cheap and portable, with potential applicability for monitoring trace-level amounts of Cd within environmental or potable water.