Magnetic microwires can present excellent soft magnetic properties and a giant magnetoimpedance effect. In this paper, we present our last results on the effect of postprocessing allowing optimization of the magnetoimpedance effect in Co-rich microwires suitable for magnetic microsensor applications. Giant magnetoimpedance effect improvement was achieved either by annealing or stress-annealing. Annealed Co-rich presents rectangular hysteresis loops. However, an improvement in magnetoimpedance ratio is observed at fairly high annealing temperatures over a wide frequency range. Application of stress during annealing at moderate values of annealing temperatures and stress allows for a remarkable decrease in coercivity and increase in squareness ratio and further giant magnetoimpedance effect improvement. Stress-annealing, carried out at sufficiently high temperatures and/or stress allowed induction of transverse magnetic anisotropy, as well as magnetoimpedance effect improvement. Enhanced magnetoimpedance ratio values for annealed and stress-annealed samples and frequency dependence of the magnetoimpedance are discussed in terms of the radial distribution of the magnetic anisotropy. Accordingly, we demonstrated that the giant magnetoimpedance effect of Co-rich microwires can be tailored by controlling the magnetic anisotropy of Co-rich microwires, using appropriate thermal treatment.