Hypothesis: Particle space arrangement is a very important factor that determines the physico-mechanical properties of soil. Formations of three-dimensional (3D) structured networks within gelled or flocculated suspension may prevent clay particles and aggregates from settling under gravity force and by encapsulate water within such a network, lead to poor sludge dewatering. To better understand this phenomenon, a microstructural investigation of a smectite clay (SWy2) suspension was conducted. Experiments: SWy-2 was diluted in water and a moderately salty aqueous solution and was studied with the aid of a synchrotron-powered transmission X-ray microscope (TXM) and cryogenic transmission electron microscope (Cryo-TEM). Observations of mutual particle arrangement in 3D spaces were conducted within a natural water environment after vitrification without drying. Findings: A new type of micro-architecture in particle space arrangement was observed. Smectite flakes were mostly in edge-to-edge (EE) contact and formed a 3D network, confirming a "net of flakes" structural model. Clay particles form a complex and multi-hierarchic flocculated structure with characteristic cellular chained networking. Chained aggregates build cellular elements, encapsulating water inside closed voids. Increasing ionic strength results in the development of multi-hierarchic voids categories, with most water retained within nano-pores. (C) 2014 Elsevier Inc. All rights reserved.