Tryptophan (Trp) is one of the essential amino acids in human body, which is important for human health. Therefore, convenient strategies for the detection of Trp are very significant. Coordination polymers (CPs) have presented great importance as fluorescent sensors in recent years. Herein, two Cd(II) CPs were synthesized as fluorescent sensors for turn-on and red-shift sensing of tryptophan, namely, {[Cd(1,4-bbix)2(1,5-NDS)]·(H2O)2}n (1) and {[Cd(bmbp)2(H2O)2]·(1,5NDS)(H2O)4}n (2), (1,5-NDS = 1,5-naphthalenedisulfonate, 1,4-bbix = 1,4-bis(benzimidazol-1-yl-methyl)benzene, bmbp = 4,4′-bis(2-methylimidazole-1-yl-methyl)biphenyl). 1 shows a three-dimensional (3D) structure with 6-connected pcu topology. 2 shows a 1D chain, which is connected by hydrogen-bonds to form the 3D supramolecular structure. Both CPs can effectively detect Trp via fluorescence enhancement and red-shift in aqueous solution with the limits of detection being 1.11 μM and 0.69 μM for 1 and 2, respectively. Two CPs also can be applied for the detection of Trp in milk with good sensitivity. The sensing mechanisms toward Trp were investigated via experimental and theoretical calculation methods. The test films were prepared for the visual detection of Trp.