Macrophages have multiple functions in modulating the physiological process, and the regulation of macrophage is essential for the design of biomaterials. Based on the special interaction between glucomannan (GM) and macrophages, in the study, GM based immunomodulation biomaterials were prepared. During the process of tissue repair, growth factors (GFs) which are important in promoting angiogenesis are mainly expressed by macrophages. But the loss of extracellular matrix components in some diseases lack the capacities for stabilizing macrophages and GFs. We designed an injectable hydrogel scaffold aiming to stimulate the secretion of endogenous pro-angiogenic GFs and sequesters them to promote in situ angiogenesis. GM which has demonstrated to have the capacity of activating macrophages/monocytes were used as the framework of the scaffold; and heparin, a representative glycosaminoglycan molecule that binds numerous pro- angiogenic GFs, was used as functional moieties to sequester the macrophage- produced GFs. By modifying with tyramine (TA) groups, the two components can be co-polymerised and rapidly form into hydrogel mediated by the enzyme. Without the addition of any exogenous GFs, the designed GM-TA/Hep-TA hydrogel could successfully promote in situ angiogenesis in the mice model. Switching "pro-tumor" macrophage back to an "anti-tumor" state is crucial for activating both the innate and adaptive immunity in cancer immunotherapy. However, commonly used agents that target macrophages have high toxicity and low specificity. Inspired by the immunostimulatory microbial signals, we summarized the two key features of pathogen-associated molecular patterns (PAMPs), which are the type of polysaccharide and the existence of the aliphatic group. By mimicking the structure of PAMPs, GM was chosen and modified with the simplest aliphatic group-acetyl group. The results showed that acetylated GM with a degree of substitution of 1.8 (acGM- 1.8) presented homogenous particulate form in a physiological environment. And it could induce macrophages into a solid anti-tumor phenotype via specifically activating toll- like receptor 2 (TLR2) signaling. Its antitumor efficiency was proved by two tumor models in mice, and its higher safety compared to four classical TLR agonists was evaluated by high dose-intraperitoneal injection. The study evaluated the potential of glucomannan derivatives in regulating macrophage behaviors by offering various patterns and bio-interfaces. The "week" stimulation in promoting angiogenesis and the "strong" stimulation in tumor immunotherapy were both successfully verified. These efforts may expand the potential of GM in preparing biomaterials and provided an innovative insight into the application of polysaccharides in immuno-regulations.