We have successfully prepared and structurally characterized triangle-in-triangle {Cr3Ln3} complexes with Ln = Gd and Dy employing alcohol-amine, N-methyldiethanolamine (H2mdea) and pivalate ligands. These complexes and the Yttrium analogue proved to be isostructural and crystallized in a P1 triclinic cell. DC and AC magnetic measurements were carried out and supported by quantum computations at DFT and CASSCF levels. DC magnetic data are dominated by the Cr(III)-Ln(III) antiferromagnetic interaction and by single-ion anisotropy in the case of the Dy(III) complex. Ln(III)-Ln(III) magnetic interactions are negligible, as well as Cr(III)-Cr(III) ones. From AC data, slow relaxation of the magnetization is observed at 0 DC applied magnetic field in the case of the Dy(III) complex below 4 K. From temperature and field dependence data, possible Raman and Orbach relaxation mechanisms are established in the absence of quantum tunnelling pathways, suggesting a successful suppression of the latter due to the Cr(III)-Dy(III) exchange interaction.