The Young's modulus of cross-linked poly(dimethylsiloxane) (PDMS) surface was quantitatively investigated as a function of UV/ozone treatment time across different length scales. An AFM was used to probe PDMS surface mechanical properties at the nanometer length scale. The Young's modulus of each sample was estimated with continuum contact mechanics theory (Sneddon method) using AFM data by employing the hyperboloid tip shape model. A custom-built ATD device (JKR method) was also used which allowed LIS to simultaneously monitor the load, the contact area, and the relative displacement between (a) a lens (made either of PDMS elastomer Or Of Si3N4) and (b) surface-treated PDMS films upon loading and unloading oil the micrometer to submillimeter length scales. The modulus of PDMS increased with increasing treatment time as observed by AFM as well as by ATD, which we explained by the gradual formation of,I silica-like layer. For all specimens tested, the modulus values obtained were highest from AFM, lower from ATD, and lowest from bulk tensile experiments for the same UV/ozone dose. These results demonstrate the effect of the probed length scale of the tests used to assess mechanical performance.