Artificial cartilages build up a highly lubricious system with the harmony of biomacromolecules and water. Bioconjugate thin films composed of a zwitterionic poly(carboxybetaine methacrylate) (PCB) brush platform and bovine serum albumin (BSA) were designed. BSA conjugation to the PCB brush chains was achieved by carbodiimide chemistry to give PCB brush/BSA conjugate films. The PCB brush/BSA conjugate films exhibited adaptable interfacial properties due to the amphiphilic nature of BSA. Neutron reflectivity showed that BSAs were localized at the liquid side of the conjugate films in PBS and the BSA conjugation slightly reduced the water content of the top layer, while the swollen state of the carpet PCB brush layer remained unchanged. The PCB brush/BSA conjugate films showed improved lubricity in the boundary lubrication mode but slightly worse fluid lubrication induction properties. This conjugate film could be a model system for the investigation of zwitterion/protein composite interfaces and is worth developing biomaterials that require lubrication in vivo.