Not immediately. Spain isn't a direct threat to France (and the British can't really launch a land invasion of France via Spain due to insane logistics). Russia is a direct threat to France once it mobilises enough, because it has the potential to turn Austria and Prussia against the French as soon as Napoleon stops looking so threatening.
Few considerations:
(a) Russia could not "mobilize enough" because its ability to do so had been limited both by its recruit-based system (in 1812 3 "recrutsky nabor" with total of 20 men from every 500 which was rather extraordinary; usually it was 1 - 5 men from 500) as opposite to the universal military system in France and economic considerations. Taking into an account that Russia had overall smaller population (in 1800 France 44,596,000 and Russia 35,005,000) a much less effective mobilization system meant a
MUCH lesser army. Its military budget already skyrocketed (and big part of the cost had been ultimately paid by the nobility) and could not keep growing forever even with the British subsidies. Even dressing and arming the increased number of troops was problematic: in 1812 some of the newly raised contingents had been arriving to the front without the weapons and uniforms because Russian industries were not up to the task.
(b) Short of a spectacular victory and clear weakening of Napoleon Prussia would not change sides and Austria would be even less inclined to do so.
(c) Prior to 1812 Alexander had only the defeats to his international "credit" and the same goes for prestige of the Russian army (if outcome of the Battle of Eylau could be disputed, Friedland was unmitigated disaster).
(d) While some of the Russian pre-1812 plans included the offensive component, they were mostly concentrating on the defensive operations.
(e) Russian army had a shortage of the experienced officers and general and on the top level situation was almost catastrophic: few very old generals and 3 capable commanders of the somewhat younger generation, Bennigsen, Bagration and Barclay, hated each other guts (as was convincingly demonstrated in 1812).
Launching an aggressive campaign in that situation, even with a hope that
may be Prussia is going to change sides, would be a recipe for disaster (especially taking into an account that inj 1812 Alexander kept meddling into the military affairs with the disastrous results being avoided just because he freaked out and left the army).
Napoleon's best move (and ultimately, the only one that will get him a victory) is to convince both Russia and Britain to stop fighting him. In early 1812 he was at the height of his power, and had already achieved everything that he could reasonably want, and that logistics would allow. And everyone was actually scared of him still.
Actually, he was trying really hard with Alexander but it did not work out. Of course this was partially Nappy's fault but Alexander did not want peace either.
So how to achieve it? With Russia, convincing the Tsar to make a lasting agreement, of anything from a non-aggression pact (for say 10 years) up, will effectively accomplish this.
One would think that Tilsit was an attempt to do just that. But as soon as Russia recuperated from a defeat Alexander started preparing for the war. It was combination of his general Anglophilia, personal hate of Napoleon and Russian economy being traditionally oriented toward Britain (the last factor could be dealt with but not with two other factors in place).
Failing that, an invasion with a decisive battle will also work. Napoleon's plan to invade Russia was sound, the only problem was that he never caught the Russian army and chased it far beyond where he should have.
In other words, short of a complete Russian incompetence, this option was impractical.
With Britain, it is just a matter of convincing them that they can't defeat France and that they might as well end the effectively 20-year long war that they were already getting sick of.
For this he would need combination of 2 things: (a) a crushing defeat of the British forces in Spain & Portugal (loss of prestige, national morale is sinking, etc.) and (b) there should be no continental suckers (Russia in this case) ready to fight for the British money. Alexander should go the same way as his father and probably the same goes for Constantine leaving 16 years old Nicholas as an Emperor of a rather confused empire.