There's maybe some very complex grammatical reason, but it may be easier to study them as collocations. Sometimes the certain preposition that is used with a certain verb or sentence structure is almost arbitrary.
A person is ‘investigated FOR something/doing something,’ whereas a person is ‘accused/suspected OF something/doing something.’ It's the same for English speakers when we try and learn Slavic languages–some verbs almost arbitrarily use a certain case or a preposition.
When ‘suspect’ is in noun form, we just arbitrarily use ‘IN.’ ‘He is the suspect IN the commission of a crime/in the robbery/in the arson case.’
When it's the verb form of ‘suspect,’ OF is used: the person is ‘suspected OF committing a crime/of wrongdoing/ of stealing a car, etc.’
Practically, it's just different ways to formulate the same kind of sentence. Out of curiosity, it looks like in Russian and Ukrainian, when talking about a person being a suspect/suspected of smth, the thing they're suspected of stays in the same case and with the same preposition. But, maybe it could be expressed analogously to the noun/verb formulations in English:
Suspect as a noun: Он является подозреваемым в совершении преступления / Він є підозрюваним у скоєнні злочину.
Suspect as a verb: Его подозревают в совершении преступления. / Його підозрюють у скоєнні злочину.