The mechanical properties of molded pulp materials are the basis of the structural optimum design of molded pulp products. Therefore, the correlations between Poisson’s ratio and fiber structure, molding process, and thickness were found for materials including wood pulp, bamboo pulp, sugarcane pulp, white mixed pulp, black mixed pulp, recycled corrugated board pulp, and recycled newspaper pulp by the uniaxial tensile test and digital image correlation method. The fiber structures of the selected molded pulp materials were investigated by scanning electron microscopy. The results revealed Poisson’s ratios of wood pulp, bamboo pulp, sugarcane pulp, white mixed pulp, black mixed pulp, recycled corrugated board pulp, and recycled newspaper pulp to be 0.169, 0.108, 0.202, 0.120, 0.166, 0.098, and 0.044, respectively. Microstructural investigation further revealed that Poisson’s ratios of molded pulp materials were related to the fiber structure and drying method. The pulp material dried outside mold under lower pressure and temperature had a smaller Poisson’s ratio, while that dried inside mold under higher pressure and temperature had a larger Poisson’s ratio. The layered phenomenon of the molded pulp materials was also found by scanning electron microscopy images: the outer layer was denser than the inner layer. These results can provide guidance for the numerical simulation analysis and optimal design of molded pulp products.