Due to the schedules being so different, it's not surprising that 9:00 might be the only time he thought he could stop by your door. I wouldn't have too much problem with that.
I wouldn't even have an issue with him offering a couple of toys for my daughter. It's a very sweet gesture and at face value, I wouldn't necessarily assume bad intentions or an ulterior motive. However, I haven't ever met him face to face so we have to rely on YOUR gut instinct. If you feel it's better not to accept any gifts from him, then you were right to refuse.
What I d have an issue with, a huge issue, is that you had to refuse more than twice. A good faith, "Oh, please take the toys, they're from my old job" is harmless until you refuse again and he continues to persist... and persist... and persist. That persistence and refusing to take "no" for an answer over something so simple as a child's toy and not being able to read your anxiety, not being able to back off and ease your anxiety, not being able to check himself... then not just being annoyed but angry and showing that anger?
I wouldn't feel guilty over accepting the first gift. You have no reason for guilt.
What I would love for you to do is find your voice and your confidence. Be certain of yourself when he offers you something or asks you to do something. Practice saying no and "no thank you" in a strong and firm voice. Practice direct eye contact, which you can do even through a chain-locked door.
"I'm not comfortable taking gifts. I would also appreciate it if you didn't come by unannounced again. Thank you. Good bye."
"I'm beginning to feel uncomfortable and would hate to have to talk to our landlord. I would prefer it if we could simply go our own ways while we're neighbors. Thank you. Good bye."
And not for nothing, but you don't have to answer your door at any time at all unless you know who it is and are expecting them willingly. There's no set of manners that says you MUST answer your door unwillingly even if the person knocking knows you're home.
If things get to uncomfortable for you, talk to your landlord. I would be interested to know how other female tenants have handled him.