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In this paper, we are relating a significant improvement of the SERS effect achieved with assembled Au/ZnO nano-urchins. This improvement is realized thanks to an excellent capacity of adsorption (denoted <i>K</i>) for thiram molecules on these plasmonic nano-urchins, which is a key point to be taken into account for obtaining a SERS spectrum. Moreover, this outlook may be employed for different types of plasmonic substrates and for a wide number of molecules. We studied the capacity of the assembled Au/ZnO nano-urchins to be sensitive to the pesticide thiram, which adsorbs well on metals via the metal–sulfur bond. For the thiram detection, we found a limit concentration of 10 pM, a value of this capacity of adsorption (<i>K</i>) of 9.5 × 10<inline-formula><math xmlns="http://www.w3.org/1998/Math/MathML" display="inline"><semantics><msup><mrow></mrow><mn>6</mn></msup></semantics></math></inline-formula> M<inline-formula><math xmlns="http://www.w3.org/1998/Math/MathML" display="inline"><semantics><msup><mrow></mrow><mrow><mo>−</mo><mn>1</mn></mrow></msup></semantics></math></inline-formula> and a factor of analytical enhancement equal to 1.9 × 10<inline-formula><math xmlns="http://www.w3.org/1998/Math/MathML" display="inline"><semantics><msup><mrow></mrow><mn>8</mn></msup></semantics></math></inline-formula>.