We have authenticated the molecular and crystal structure of (ZnBu2)-Bu-t and constructed the unprecedented 2D fabric structure using the tert-butylzinc molecules and 1,2-bis(4-pyridyl)ethane as building blocks. The X-ray crystal structure analysis revealed that the inorganic-organic polymeric chains were weaving to form the fabric structure by the concerted C-H center dot center dot center dot pi interactions involving the pyridine rings. Subtle factors governing self-assembly processes leading to a fabric structure are discussed.