Calcium polyphosphate (CPP) is a new type of degradable material for bone repair, yet it is fragile and is not so controllable in regard to degradation. For increasing biological activity and close proximity to natural bone structure, in this experiment, we chose chitosan (CS) and its derivative carboxymethyl chitosan (CMC) as the extracellular matrix structure for the organic phase. Aldehyde sodium alginate (ADA) was used as natural cross-linker. The binary (CPP/CMC) and ternary (CPP/CMC/CS) composite scaffolds were prepared by the "multiple composite-cross-linking method". The degradation laws of the two materials were investigated through the weight loss of scaffolds, the pH value of degradation solution, the compressive strength and the surface morphology characterization. The results showed that the composite scaffolds had good interface and the compressive strength increased greatly, but the organic phase of dual-phase composite scaffolds degraded quickly, while degradation controllability and mechanical properties of ternary composite scaffold were significantly improved. All the above findings show that the method of ternary complex scaffold preparation is useful for the design and preparation of bone tissue engineering materials.