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In this paper we review recent highlights of our research on the interaction of ultrafast laser pulses with surfaces with the aim of analyzing the fundamental mechanisms during micro/nanoprocessing of the irradiated surfaces and investigate the perspectives and applications arising from the irradiation of novel complex and functional materials with simple as well as temporally modulated femtosecond laser pulses. Our results on the irradiation of Si and ZnO surfaces show that the crater size and the ripple formation can be controlled by irradiation with properly temporally shaped laser pulses. Together with simulations of the dynamics of the phase changes of the material’s surface we show the potential for understanding and tailoring the engineering of smart optical materials at the micro- and nanoscale intended for novel optoelectronic applications and devices.