AbstractHerein, two electrochemical methods based on potentiometric and impedimetric transductions were presented for albumin targeting, employing screen‐printed platforms (SPEs) to make easy and cost‐effective sensors with good detection merits. The SPEs incorporated ion‐to‐electron multi‐walled carbon nanotubes (MWCNTs) transducer. Sensors were constructed using either tridodecyl methyl‐ammonium chloride (TDMACl) (sensor I) or aliquate 336S (sensor II) in plasticized polymeric matrices of carboxylated poly (vinyl chloride) (PVC‐COOH). Analytical performances of the sensors were evaluated using the above‐mentioned electrochemical techniques. For potentiometric assay, constructed sensors responded to albumin with −81.7 ± 1.7 (r2 = 0.9986) and −146.2 ± 2.3 mV/decade (r2 = 0.9991) slopes over the linearity range 1.5 μM–1.5 mM with 0.8 and 1.0 μM detection limits for respective TDMAC‐ and aliquate‐based sensors. Interference study showed apparent selectivity for both sensors. Impedimetric assays were performed at pH = 7.5 in 10 mM PBS buffer solution with a 0.02 M [Fe(CN)6]−3/−4 redox‐active electrolyte. Sensors achieved detection limits of 4.3 × 10−8 and 1.8 × 10−7 M over the linear ranges of 5.2×10−8–1.0×10−4 M and 1.4×10−6–1.4×10−3 M, with 0.09 ± 0.004 and 0.168 ± 0.009 log Ω/decade slopes for sensors based on TDMAC and aliquate, respectively. These sensors are characterized with simple construction, high sensitivity and selectivity, fast response time, single‐use, and cost‐effectiveness. The methods were successfully applied to albumin assessment in different biological fluids.