Hydrosilylation is one of the largest-scale applications for homogeneous catalysis and is widely used to enable the commercial manufacture of silicon products. In this paper, a bifunctional heterogeneous catalyst, Pt^δ+/AET-MIL-101 (AET = 2-aminoethanethiol) with a partially positively charged Pt^δ+ electronic structure is reported, which was successfully prepared using post-synthesis modification with AET and a platinum precursor. The catalysts were characterized using X-ray diffraction (XRD), nitrogen (N₂) adsorption–desorption, transmission electron microscopy (TEM), scanning electron microscopy (SEM) and X-ray photoelectron spectroscopy (XPS) techniques which showed that the synergy of AET-MIL-101 provides a good dispersion of Pt^δ+ in the channels, which can efficiently catalyze the hydrosilylation reaction with almost complete conversion and produce a unique adduct. In addition, the synthetic heterogeneous catalyst Pt^δ+/AET-MIL-101 achieves reasonable use of Pt in terms of number cycles and atomic utilization efficiency, indicating the potential to achieve a green hydrosilylation industry.