In this work, we report on the synthesis of Ge nanocrystals (NCs) by pulsed laser deposition (PLD) at room temperature (RT) in an argon atmosphere without any further annealing process. Our results show that functional thin films of crystalline Ge nanoparticles with spherical shapes can be obtained by PLD directly on alumina layers deposited on n-doped Si (100) substrates. In addition, we also demonstrate that a uniform size distribution of NCs with an average diameter of about 3 nm and a density of 2.3 × 1011 cm−2 can be obtained by optimizing a shadow mask set-up, where a solid disk is introduced between the target and the substrate. Charge/discharge effects in Ge NCs deposited on a high-k amorphous alumina layer are also evidenced by conductive atomic force microscopy, which makes them suitable for memory applications.