Improved matrix or hydrogel that is formed by enzymatic crosslinking of polymers wherein the crosslinking enzyme molecules have been modified for the purpose of improving the crosslinking density, mechanical properties, or other properties of the matrix, and/or to provide improved control over the rate and/or extent of crosslinking, wherein the enzyme molecules are modified to alter the perceived volume of the enzyme molecules in the crosslinked matrix being formed. Methods of production and of use are also provided.