Throughout the 1920s and 1930s, in addition to his successful business career, Simonsen became one of the country's main industrialist leaders. His projection on the national public stage began in 1919, when, at the invitation of the then Minister of Agriculture, he was part of the trade mission sent to England in June of that year. On this occasion, Simonsen became actively involved in the debates, gave speeches asking for technical support for the Brazilian economy and wrote articles for the Times Magazine disseminating business opportunities in Brazil. Throughout the 1920s, Simonsen took part in the industrial diversification movement then underway, becoming president of the Sindicato Nacional dos Combustíveis Líquidos [National Liquid Fuels Union] in 1923. In 1924, he was the director of Cerâmica São Caetano [São Caetano Ceramics] and, in 1926, he organised the national rubber and copper artifacts campaigns. A landmark moment in his career as a business leader dates back to 1928, when, faced with disagreements between industrial and commercial interests within the Associação Comercial de São Paulo [São Paulo Trade Association], he took part in the founding of the Centro das Indústrias do Estado de São Paulo [São Paulo State Industries Centre] (CIESP, later named FIESP) and became its vice-president. The speech he gave at the founding of CIESP, published under the title "Orientação Industrial Brasileira" [Brazilian Industrial Orientation], is regarded as a milestone in Simonsen's political and intellectual career. On that occasion, he introduced a series of topics that would be explored in greater depth throughout the 1930s and 1940s, particularly the assertion of industry’s indispensability for the country’s economic and political independence, the challenge to the concept of "artificial industry" (which was used to dismiss protectionist policies), and the advocacy for more extensive protectionist measures.

In the 1930s, Simonsen's involvement in the public sphere became more and more prevalent. In 1932, he became actively involved in the creation of the Frente Única de São Paulo (FUP), which demanded political autonomy for the state and the immediate reconstitutionalisation of the country. Once the armed struggle broke out in July of that year, he was one of the main people responsible for adapting São Paulo's industrial park to the war economy. Once the civil war was over, the Vargas government was forced to convene a Constituent Assembly, which led Simonsen to be nominated as a member of parliament, and he was reappointed to the same position in 1934. Between 1935 and 1936, Simonsen chaired the Centro Industrial do Brasil [Industrial Centre of Brazil] (CIB) and, in 1937, was elected president of FIESP, consolidating his position as Brazil's main industrialist leader.

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