Nanometer-scale patterning and charging in layer-by-layer (LbL) ultrathin films of quinquethiophene (5TN)/phthalocyanine (CuPS) provides a novel write-read device using a standard current-sensing atomic force microscopy (CS-AFM). The AFM height images showed dented or raised morphological features that could be selectively manipulated by changing the direction of the bias voltages. The conductivity was repeatedly changed between a conductive and insulating state, originating from an electrochemical charging-discharging effect. This was attributed to electrochemical ion transport and the residual mobile ions present in LbL films. Finally, the nanocharge pattern was written by CS-AFM and read out in a conductivity map image.