Textured heterogeneous surfaces and related articles as can be used in conjunction with methods for selective sensing and/or separation. When used for selective particle separation such a system can comprise a heterogeneous surface comprising a surface member and a plurality of components extending therefrom, such components spaced about and having a surface density, with heterogeneity comprising different interactions of the surface member and of the extended components with a particle exposed thereto. Various surface heterogeneities and different interactions can be utilized. However, in certain embodiments, competing electrostatic interactions, or a combination of electrostatic and non-electrostatic interactions, with a particle can be utilized. Such a system can utilize a surface member having a charge difference with respect to the components extending therefrom.