Born in Paris to a father who worked as the motoring correspondent for the Petit Parisien newspaper, Wimille developed a passion for racing from an early age. He made his Grand Prix debut at age 22, driving a Bugatti 37A at the 1930 French Grand Prix in Pau. Early results followed quickly: in 1931 he finished second at the Monte Carlo Rally driving a Lorraine-Dietrich, and in 1932 he won the La Turbie hill climb, the Grand Prix de Lorraine, and the Grand Prix d'Oran in a Bugatti T51.
Through the mid-1930s Wimille established himself as a front-rank driver in the Bugatti team. He won the 1934 Algerian Grand Prix in Algiers and the 1936 French Grand Prix, the latter in an accident-marred Deauville street race that killed two other drivers, Raymond Chambost and Marcel Lehoux, leaving only three of the original sixteen starters to finish. That same year he competed at the Vanderbilt Cup on Long Island, finishing second to Tazio Nuvolari.
His greatest prewar achievements came at Le Mans. In 1937 he shared a Bugatti T57G with Robert Benoist to take overall victory; in 1939 he won again, this time co-driving a Bugatti Type 57C with Pierre Veyron. These back-to-back Le Mans victories placed him among the most accomplished endurance drivers of the decade.
With the outbreak of war in 1939 Wimille joined the French air force, but was demobilized following France's defeat in June 1940. In late 1943 he was recruited by fellow racing driver Robert Benoist into the British Special Operations Executive as an agent within the Clergyman network, which was based near Nantes. Benoist, Wimille, wireless operator Denise Bloch, and other operatives successfully destroyed several power line pylons. William Grover-Williams also participated in the resistance alongside them.
On 18 June 1944 the Germans raided Benoist's chateau near Sermaise, Essonne and captured several Clergyman members including Bloch. Wimille escaped into the surrounding forest and concealed himself beneath the roots of a tree overhanging a small stream, keeping only his head above water until the Germans departed. He then sheltered at a nearby farm and eventually made his way to Paris. Wimille's companion and future wife Christiane de la Fressange — a former member of the French national ski team — was among those captured but escaped in August 1944 while being transported by train to a German concentration camp. Benoist and Grover-Williams were both ultimately captured and executed; Wimille was the only one of the three SOE drivers to survive the war.
After Paris was liberated in August 1944, Wimille flew reconnaissance missions with the French air force until the end of hostilities in May 1945.
Wimille resumed racing in 1946 as the number-one driver for the Alfa Romeo works team, a position he held through 1948. Driving the supercharged Alfa Romeo 158, he won the Coupe de la Résistance, the Grand Prix des Nations in Geneva, the 1947 Swiss Grand Prix, the 1947 Belgian Grand Prix, the 1948 French Grand Prix, and the 1948 Italian Grand Prix, among others. His postwar results arguably made him the fastest driver in the world before the inaugural Formula One World Championship season of 1950, which he did not live to contest.
Alongside his racing commitments, Wimille designed and built cars under his own name in Paris between 1946 and 1950. Around eight cars were constructed in total, initially using Citroën engines and later Ford V8 units. He also collaborated with Marcel Lesurque on an electric car capable of reaching 50 km/h, a project begun during the war years in 1940.
During practice for the 1949 Buenos Aires Grand Prix, Wimille lost control of his Simca-Gordini and crashed into a tree. He was 40 years old. He is buried in the Cimetière de Passy in Paris; a memorial stands at the Porte Dauphine on the edge of the Bois de Boulogne.
Wimille is remembered as perhaps the most complete French racing driver of the prewar and early postwar eras — equally dominant in Grand Prix racing and endurance events — and as a man of genuine courage whose wartime resistance activities placed him at serious personal risk. His dual legacy as champion and resistance fighter remains a defining part of his reputation in French motorsport history.