Alongside ghostwriter Don Moore, a pulp-fiction veteran, Raymond created the visually sumptuous science-fiction epic comic strip Flash Gordon. The duo also created the "complementary strip, Jungle Jim, an adventurous saga set in South-East Asia", a topper which ran above Flash in some papers. Raymond was concurrently illustrating Secret Agent X-9, which premiered January 22, 1934, two weeks after the two other strips. It was Flash Gordon that would outlast the others, quickly "developing an audience far surpassing" that of Buck Rogers. Flash Gordon, wrote Stephen Becker, "was wittier and moved faster," so "Buck's position as America's favorite sci-fi hero", wrote historian Bill Crouch, Jr., "went down in flames to the artistic lash and spectacle of Alex Raymond's virtuoso artwork." Alex Raymond has stated, "I decided honestly that comic art is an art form in itself. It reflects the life and times more accurately and actually is more artistic than magazine illustration—since it is entirely creative. An illustrator works with camera and models; a comic artist begins with a white sheet of paper and dreams up his own business—he is playwright, director, editor and artist at once." A. E. Mendez has also stated that "Raymond’s achievements are chopped into bite-sized pieces by the comic art cognoscenti. Lost in the worthwhile effort to distinguish comics as an art form, the romance, sweep and beauty of Raymond's draftsmanship, his incomparable line work, is dismissed. To many, it's just pretty pictures. Somehow or another, it's OK for people like Caniff and Eisner to borrow from film. That’s real storytelling. But for Raymond to study illustrators, well, that's just not comics."

Debuting on January 7, 1934, Raymond's first Flash strip introduced the "world-famous polo player", improbably roped into a space adventure alongside love-interest Dale Arden and scientist Dr. Hans Zarkov. Transported by rocket to the planet Mongo, "which was about to collide with Earth", the trio "immediately became embroiled in the affairs of Mongo's inhabitants...particularly those of its insidious warlord, Ming", who would become Flash Gordon's nemesis throughout the franchise's many incarnations.

The first Flash Gordon and one from 1936 show how Raymond expanded from the standard layout to larger panels.

Raymond's sensual artwork—for which the artist particularly "studied popular illustrators," including pulp artist Matt Clark, whose work Raymond's male figures particularly evoke—outshone its borders and "attracted far more loyal readers than...the rather contrived and unconvincing adventure stories" his work depicted. Raymond swiftly became "among the most highly-regarded—and most imitated—in all of comics" for his work on the weekly strip, with Harvey declaring his work on the strip "a technical virtuosity matched on the comics pages only by Harold Foster in Prince Valiant." Raymond evolved the layout of the strip from a four-tier strip in 1934 to a two-tier strip in 1936, reducing the number of panels but doubling their size. Combining this with a removal of dialogue from speech balloons to captions at the bottom of the panel afforded Raymond the space to create detailed and atmospheric backgrounds. Against these spacious backgrounds, the placement of characters in heroic pose "lent the entire enterprise a mythic air."

Flash Gordon gained a daily strip in 1940, illustrated by Austin Briggs. Raymond left the Sunday strip in 1944 to join the Marines, whereupon the daily strip was cancelled and Briggs assumed Sunday duties, continuing until 1948. Briggs was succeeded on the Sundays by Emanuel "Mac" Raboy, while the daily strip was revived in 1951 by Dan Barry. Barry also took over Sunday duties after Raboy's death in 1967.

Run above Flash Gordon, Raymond's Jungle Jim is described by Armando Mendez as "a thing of beauty... always more than just a topper or a shallow response to Hal Foster's exquisite Tarzan". The companion strip evolved over time, morphing from an initial "two tiers and up to six panels [layout], with speech balloons" into "a single row, of four very tall panels with declamatory text and static, vertical composition". Raymond's skill and artistic dexterity, however, kept the storytelling constant and the artwork vibrant. Jungle Jim was "set in contemporary times and the exotic Malay peninsula of islands, but was intended to hark back to the original tales of Kipling, Haggard and Burroughs".

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