Chirality is an important and fascinating concept which has not been properly addressed in carbon nanoscience [1]. We have previously reported the first inherently chiral bilayer nanographene with a helicene linker, both as the racemate and the M isomer [2,3]. Helical bilayer nanographenes (HBNGs) are chiral π-extended aromatic compounds consisting in two π-π stacked hexa-benzocoronenes (HBC) joined by a helicene, thus resembling van der Waals layered 2D materials. Recently, we have synthesized and compared [9]HBNG, [10]HBNG and [11]HBNG helical bilayers endowed with [9], [10] and [11]helicenes embedded in their structure, respectively. Interestingly, the helicene length defines the overlapping degree between the two HBCs (number of benzene rings involved in π-π interactions between the two layers), being of 26, 14 and 10 benzene rings, respectively, according to the X-ray analysis [4]. More interesting, this overlapping also controls the properties.Compounds constituted only by carbon atoms, such as optically active molecular nanographenes have, so far, been obtained as racemates followed by time-consuming chiral chromatographic separations. In this presentation, an enantioselective strategy of a new bilayer nanographene which uses two pivotal stereocontrolled key synthetic steps to introduce and extend stereogenic elements into a polycyclic aromatic Csp2-based structure will be discussed. The resulting helical core of six ortho-fused rings embedded in the nanographene ensures stereochemical stability and good chiroptic activity [5]. Acknowledgements : This work has been supported by the Ministerio de Educación, Cultura y Deporte of Spain (Grant PID2020-114653RB-100).