This study concerned an amorphous surface layer on blown polyethylene film with a composition different from that of the bulk. The surface layer was characterized by gentle probing with an atomic force microscope. The demonstration of an amorphous layer uniformly covering the surface of a blown Ziegler-Natta-catalyzed polyethylene (znPE) film reproduced previous reports. Removing the surface layer by solvent washing confirmed the hypothesis that the layer consisted of lower molecular weight, higher branch content fractions. A blown film of znPE blended with up to 30 wt % impact-modified high-melt-strength polypropylene (hmsPP) also exhibited an amorphous surface layer. In thin films, it was advantageous for the mobile, amorphous fractions of ethylene-propylene rubber (EPR) to locate at the surface rather than at the phase interface. The amorphous EPR tended to segregate into pools on the film surface, and this pointed to a substantial difference between the amorphous surface layers on the znPE and hmsPP/znPE blend films. Surface enrichment best described the compositional gradient that resulted from the concentration of lower molecular weight, higher branch content chains at the surface of the znPE film. Surface segregation was more appropriate for the emergence of EPR fractions as a separate phase on the surface of the hmsPP blend film. Films blown from a blend of a Ziegler-Natta-catalyzed polyethylene and a metallocene-catalyzed polyethylene (zn/mPE) and its blend with hmsPP reproduced the primary features of surface enrichment and surface segregation. Some differences between the znPE and zn/mPE films were attributed to the metallocene constituent of zn/mPE.