The title of Crime and Punishment fits the narrative and the themes because both the narrative and the themes are about crimes committed and punished or not punished. Let me clarify a little for you.Several characters commit crimes of varying sorts who are or are not punished for them.
An example of this is when Dounia shoots Svidrigailov for his attempted crimes against her. In so doing, she commits a crime. Yet she will not be punished for it because Svidrigailov will say nothing. Guilt from this incident and his other crimes weigh him down until he ends his life in shame and despair.
she raised the revolver ... and there was a pang of [desire] in his heart. He took a step forward and a shot rang out.
Other characters commit moral crimes that are not legal crimes. Two of these are Marmeladov and Luzhin. Each brings shame and suffering on the woman they desire, Marmeladov against Katerina Ivanovna a great more severely than Luzhin against Dounia, though. These characters may be "punished" by circumstances such as when Marmeladov dies so helplessly, yet this punishment leaves his victims in worse and more direful straits than before.
An example of this kind of crime is Sonia. She is forced as a result of Marmeladov's moral crimes to accept being registered for a "yellow ticket" that allows her to commit the crime of prostitution without fear of punishment.
Sonia ran to restrain Katerina Ivanovna, but when Amalia Ivanovna shouted something about "the yellow ticket,"
The title most significantly applies to Raskolnikov, of course since he is the one who commits the heinous crime against Alyona Ivanovna, "the old lady." And it is Raskolnikov whom the police pursue and catch. It is Raskolnikov who is punished in a Siberian prison camp for his crime.
"Will you come and see me in prison when I am there? [...] Sonia, you'd better not come and see me when I am in prison." (Raskolnikov to Sonia)
Now you can see that the title is perfectly suited to the narrative because in it Dostoevsky explores many forms and degrees of crimes committed against other persons and punishment meted or escaped for the crimes. We mentioned a few instances, but there are others, like Luzhin's attempted crime against Sonia where he wrongly accuses her of crime.
"if it had suited his plans, [Luzhin] would have sent you to prison if it had not been for Lebeziatnikov and me. Ah?" (Raskolnikov to Sonia)