The capacity of a synthetic (N1E, N3E)-N1,N3-bis(quinolin-2-ylmethylene)benzene-1,3-diamine Schiff base ligand to operate as a cation carrier in a poly(vinylchloride) (PVC) membrane (electrode I) and screen-printed ion-selective electrode (SPE) (electrode II) was investigated. The screen-printed and the fabricated poly(vinylchloride) membrane (PVC) electrodes displayed outstanding response properties for Al(III) ions. The electrodes had linear potential response with a slope of 17.95 ± 0.14 and 19.80 ± 0.46 mV decade−1 in the concentration range of 1.0 × 10−5–1.0 × 10−1 and 1.0 × 10−7–1.0 × 10−1 mol L−1 for electrode I and electrode II, respectively. The detection limit of the proposed sensors is 2.1 × 10−6 and 6.3 × 10−8 mol L−1, and it can be used over a period of 35 and 190 days for electrode I and electrode II, respectively. The suggested sensors showed strong selectivity against a wide range of other cations, including alkali, alkaline earth, heavy, and transition metals, and could be employed in pH ranges of 3.0–6.0 and 2.5–6.5 for electrode I and electrode II, respectively. The effect of several plasticizers has been studied. These electrodes had been successfully used to determine Al(III) in aqueous solution and various real water samples. They used as an indicator electrodes in aluminum ion potentiometric titration against standard EDTA solution. The devised approach was used to determine the concentration of Al(III) in several real water samples with high percentage recoveries and low standard and relative standard deviation values. The results were in good agreement with those obtained using atomic absorption spectrometry as indicated from the calculated t- and F-test values.