Embodiments of the invention provide a method for in-situ selective deposition and etching for advanced patterning applications. According to one embodiment the method includes providing in a process chamber a substrate having a metal-containing layer thereon, and exposing the substrate to a gas pulse sequence to etch the metal-containing layer in the absence of a plasma, where the gas pulse sequence includes, in any order, exposing the substrate to a first reactant gas containing a halogen-containing gas, and exposing the substrate to a second reactant gas containing an aluminum alkyl. According to another embodiment, the substrate has an exposed first material layer and an exposed second material layer, and the exposing to the gas pulse sequence selectively deposits an additional material layer on the exposed first material layer but not on the exposed second material layer.