Under hydrothermal conditions, two new 3D actinide–silver (An–Ag) heterometallic coordination polymers, namely, [Ag(UO2)2(µ2‐OH)(bpdc)2(H2O)2]n (1) and [Ag3Th6(µ3‐O)(µ3‐OH)(µ2‐OH)6(bpdc)6(NO3)6·H2O]n (2, H2bpdc = 2,2′‐bipyridine‐3,3′‐dicarboxylic acid), were assembled through a hard–soft recognition strategy. Compounds 1 and 2 were characterized by single‐crystal X‐ray diffraction, powder X‐ray diffraction, and infrared spectroscopy. Both compounds are constructed through the bridging of infinite polynuclear An–bpdc chiral helical chains by AgI cations. Compound 2 represents the first ThIV–AgI heterometallic coordination polymer. Furthermore, the thermal stability and luminescence properties of 1 were studied.