Composite metal–organic frameworks combine large and accessible surface areas with low density and high stability. Herein, we present novel nanocomposites of polypyrrole/aluminum fumarate metal–organic framework (PPy/AlFu MOF), which were synthesized via in situ oxidative polymerization with the aim of MOF functionalization to enhance its thermal stability and increase the specific surface area so that these nanocomposites may be used as potential adsorbents. The synthesized nanocomposites were characterized by various techniques, such as powder X-ray diffraction, scanning electron microscopy, and Fourier-transform infrared spectroscopy (FTIR). The successful functionalization of aluminum fumarate MOF was confirmed by FTIR, and the Brunauer–Emmett–Teller (BET) surface area of the PPy/MOF nanocomposite slightly increased from 795 to 809 ${\mathrm{m}}^2/\mathrm{g}$. Thermogravimetric analysis data also show that the weight loss of the composite is up to 30% at temperatures up to 500 $℃$. Remarkably, lead (50 ppm) sequestration using the composite was tested, and the atomic absorption spectrometry data demonstrate that PPy/MOF is a super-adsorbent for heavy metal ions. This work shows that the novel polymer–MOF composites are promising materials for the selective removal of lead from wastewater streams.