Limited information is available on the interaction of anionically charged lignin and cationic particles, despite the promising use of anionic lignin as a coagulant and dispersant for suspension systems. The main objective of this study was to discover the fate of lignin on its interaction with rigid and soft surfaces. In this work, carboxymethylated lignin (CML) with two different charge densities were produced, and their adsorption performance on gold and poly(diallydimethylammonium chloride) (PDADMAC)-coated gold surfaces was comprehensively studied. The viscoelastic properties of adsorbed CML on the gold surface were investigated by means of quartz crystal microbalance with dissipation. A higher adsorbed amount and compact layer were observed for the adsorption of CML with a lower charge density of -1.16 meq/g (CML1). CML with a higher charge density (-2.92 meq/g), CML2, yielded a lower surface excess density of 2.31 × 10-6 mol/m2 and a higher occupied area per molecule (71.84 Å2) at the interface of water and gold sensor. Below and at equilibrium, CML2 generated a bulkier adsorption layer than did CML1 on the gold sensor and on the PDADMAC-coated sensor. Studies on the layer-by-layer (LBL) assembly of CML and PDADMAC revealed that CML1 adsorbed more greatly than CML2 on PDADMAC, and it generated a thicker but less viscoelastic layer. In this system, the greater loss to storage modulus ( G″/ G') value was achieved for CML2, indicating its looser structure in the LBL system. Studies on the LBL assembly of carboxymethylated xylan/PDADMAC and CML/PDADMAC provided concrete evidence for the fate of three-dimensional structure of CML on its adsorption performance.