Chemical fractionation of copper in bulk soil and its distribution in the particle-size fractions were analyzed in a Cu-contaminated soil (674±122 μg Cu g−1, up to 1900 μg Cu g−1 in the clay fraction) sampled from a wood preservation site left untreated and subsequently treated with dolomitic limestone (DL, 0.2% w/w) and compost (CM, 5% w/w), singly and in combination (DL+CM). Soil enzymatic activities of leucine aminopeptidase, cellulase, N-acetyl-β-glucosaminidase, arylsulfatase, β-glucosidase, acetate esterase, butyric esterase, and acid phosphatase were determined. Chemical speciation showed that Cu was mostly present in the acid-soluble and reducible fractions in both untreated and treated soils, whereas treatments with DL and CM reduced the soluble and exchangeable Cu fractions, due to Cu precipitation and complexation, and increased Cu bound to soil organic matter. Analysis of the particle-size fractions showed that more than 80% of Cu was in the silt and clay fractions and that treatment with CM increased the concentration of Cu in the sand size fractions. Soil treatment with DL and CM, singly or in combination, increased hydrolase activities, mainly in the clay fraction, with the largest positive effects on N-acetyl-β-glucosaminidase, leucine aminopeptidase, and β-glucosidase activities. Overall, results confirm that (1) Cu in contaminated soils is mainly bound to the silt–clay fraction, (2) CM additions change its allocation in the particle-size fractions, and (3) treatments with DL and CM singly and in combination reduce Cu solubility and its inhibitory effects on soil enzyme activities.