The fact of formation of inclusion complex of C-methylresocinarene with acetone is well known. In the structure of the complex, acetone molecule is placed inside the complementary macromolecular cavity of the resorcinarene host. Moreover, complex moieties tend to aggregate into columns of the head-to-tail arrangement. The properties of C-methyl resorcinarene mentioned above have been exploited in our research on supramolecular assemblies co-formed by calixarene. By crystallization using diffusive method (acetone – water, resorcinerene and isoquinoline dissolved in acetone phase) colourless crystals of [C-methyl resor[4]arene • acetone] • tetraisoquinoline were obtained (a=34.9060, b=7.9358, c=22.6027, β=116.1031, C2/c). Indeed, columnar aggregation of the complex moieties is observed in the crystal structure, as assumed in the project. Columns are arranged side by side with antiparallel orientation thus leading to formation of layers with the (1 0 0) orientation and the distance of 15.673 Å (measured as the distance between the planes of neighboring layers, the plane is based on the carbon atoms of the carbonyl groups of the complexed acetone molecules present in given layer). Voids between the layers formed in the consequence of their packing in the crystal lattice are filled by centrosymmetric stacks consisted of four π···π interacting isoquinoline molecules. Molecules in the stack are off-set with the same orientation of the longitudinal molecular axis. The distances between centroids of the molecules in the stack are 3.931, 3.841, 3.931Å and angles between planes based on the whole aromatic system of the isoquinoline are 7.69, 0.0 7.69º respectively. Outermost component stack molecules take part also in formation of π···π interaction with phenol rings of the resorcinarene molecules belonging to opposite layers. Besides, two pairs of the isoquinoline molecules of the stack participate in formation of hydrogen bonds with two subsequent resorcinarene molecules of the layer.