Bone defects arising from trauma, disease, or surgical intervention represent significant challenges. Developing effective bone tissue engineering strategies to address these issues and promote repair is crucial. beta-Tricalcium phosphate (beta-TCP) has emerged as a promising synthetic graft due to its porous, degradable structure and excellent biocompatibility. However, the lack of biological cues in beta-TCP limits its functionality, requiring different surface modification strategies. Bone morphogenetic protein-2 mimetic peptide (BMP; NSVNSKIPKACCVPTELSAI) and collagen mimetic peptide (CMP; GTPGPQGIAGQRGVV) have a known significant therapeutic potential due to their ability to enhance cell attachment and osteogenic differentiation. Herein, a peptide functionalization strategy for beta-TCP scaffolds was introduced. Briefly, beta-TCP was treated with cold atmospheric plasma (CAP) to create functional hydroxyl groups on the surface of the beta-TCP. Subsequently, peptides were conjugated by using a three-step method: (1) silanization with APTES, (2) EDC activation, and (3) peptide conjugation. The successful surface modification with CAP and peptide conjugation was confirmed via XRD, FTIR, and Raman analysis. Furthermore, the effects of BMP and CMP peptides on osteogenic differentiation after CAP treatment were investigated in human mesenchymal stem cells (hMSCs). Both beta-TCP/BMP and beta-TCP/CMP scaffolds demonstrated excellent biocompatibility with hMSCs, enhancing cell proliferation and promoting osteogenic differentiation. Remarkably, beta-TCP/CMP showed better results in terms of proliferation and differentiation compared with beta-TCP/BMP. These findings highlight the clinical potential of peptide-functionalized beta-TCP scaffolds for bone tissue engineering while also providing a promising methodology for beta-TCP functionalization.