As an important metal element, aluminium has a significant impact on the environment and human health, and thus the detection of Al 3+ has become the subject of much research. We synthesized a Ni(II)-based metal-organic gel (Ni-MOG), which can serve as an Al 3+ fluorescence sensor with high selectivity and sensitivity, the limit of detection being calculated to be 0.5 μM. In addition, a composite film was further fabricated by hybridization of this Ni-MOG with poly(vinyl alcohol). The composite film produced a rapid fluorescence response to Al 3+ solutions at concentrations above 5 × 10 −5 M in 5 min. The Ni-MOG composite film can also be successfully applied for the sensitive detection of Al 3+ in real samples of tap water and seawater. The effective detection of Al 3+ described in this contribution provides a new insight into water quality monitoring and has promising application value.