Molecularly designed, random copolymer-bioconjugates based on poly(2-methyl-2-oxazoline) (PMOXA) and poly(2-ethyl-2-oxazoline) (PEOXA) are crosslinked in the presence of sortase A (SA) and human articular chondrocytes (hACs), to yield cellularized polymer networks. Their gelation kinetics and mechanical properties are finely tuned by varying the concentration of SA, while a cell viability >90% is achieved after several weeks of culture, even in the absence of any cell-adhesive cue.