The first examples of Wolf Type II Zn2Ln‐containing metallopolymers poly{MMA‐co‐Zn2(L)2(4‐vp)2Ln(NO3)3} (Ln = La, Nd, Yb, Er, Gd; H2L = N,N′‐bis(salicylidene)ethylene‐1,2‐diamine; 4‐vp = 4‐vinylpyridine; MMA = methyl methacrylate) are obtained from the controlled copolymerization of heterotrinuclear Zn2Ln‐arrayed complexes Zn2(L)2(4‐vp)2Ln(NO3)3 (Ln = La, 1; Ln = Nd, 2; Ln = Yb, 3; Ln = Er, 4; Ln = Gd, 5) with MMA. The strong and characteristic near‐infrared (NIR) luminescent Ln3+‐centered emission for each of the PMMA‐supported poly{MMA‐co‐Zn2(L)2(4‐vp)2Ln(NO3)3} (Ln = Nd, Yb, Er) hybrid materials is retained with somewhat higher intrinsic quantum yields than those of the respective Zn2Ln‐arrayed complex. Especially for poly(MMA‐co‐3), which has more efficient sensitization from both ligand‐centered singlet (1LC) and triplet (3LC) states of the chromophores, the concentration self‐quenching of Yb3+‐based NIR luminescence could be effectively prevented. The first examples of Wolf Type II near‐infrared‐luminescent Zn2Ln‐containing metallopolymers poly{MMA‐co‐Zn2(L)2(4‐vp)2Ln(NO3)3} (H2L = N,N′‐bis(salicylidene)ethylene‐1,2‐diamine; Ln = La, Nd, Yb, Er, Gd; MMA = methyl methacrylate; 4‐vp = 4‐vinylpridine) are obtained from the controlled copolymerization of MMA with a series of Zn2Ln‐arrayed Schiff base complexes Zn2(L)2(4‐vp)2Ln(NO3)3.