In this paper, two kinds of Be/2024Al composites were prepared by the pressure infiltration method using two different beryllium powders as reinforcements and 2024Al as a matrix. The effect of interfacial strength on the mechanical behavior of Be/2024Al composites was studied. Firstly, the microstructure and mechanical properties of the two composites were characterized, and then the finite element analysis (FEA) simulation was used to further illustrate the influence of interfacial strength on the mechanical properties of the two Be/2024Al composites. The mechanical tensile test results show that the tensile strength and elongation of the beryllium/2024Al composite prepared by the blocky impact grinding beryllium powder (blocky-Be/2024Al composite) are 405 MPa and 1.58%, respectively, which is superior to that of the beryllium/2024Al composite prepared by the spherical atomization beryllium powder (spherical-Be/2024Al composite), as its strength and elongation are 331 MPa and 0.38%, respectively. Meanwhile, the fracture of the former shows brittle fracture of beryllium particles and ductile fracture of aluminum, while the latter shows interface debonding. Further FEA simulation illustrates that the interfacial strength of the blocky-Be/2024Al composite is 600 MPa, which is higher than that of the spherical-Be/2024Al composite (330 MPa). Therefore, it can be concluded that the better mechanical properties of the blocky-Be/2024Al composite contribute to its stronger beryllium/aluminum interfacial strength, and the better interfacial strength might be due to the rough surface and microcrack morphology of blocky beryllium particles. These research results provide effective experimental and simulation support for the selection of beryllium powder and the design and preparation of high-performance beryllium/aluminum composites.